KERR ELECTRO-OPTIC MEASUREMENTS IN LIQUID DIELECTRICS by Xuewei Zhang B.S., Electrical Engineering Tsinghua University, Beijing, China, 2007 M.S., Electrical Engineering Tsinghua University, Beijing, China, 2009 Thesis Submitted to Department of Electrical Engineering and Computer Science in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy at the Massachusetts Institute of Technology June 2014 © 2014 Massachusetts Institute of Technology. All rights reserved. Author………………………………………………………………………………………………………………. Department of Electrical Engineering and Computer Science May 21, 2014 Certified by…………………………………………………………………………………………………………. Markus Zahn Thomas and Gerd Perkins Professor of Electrical Engineering Thesis Supervisor Accepted by……………………………………………………………………………………………………….... Leslie A. Kolodziejski Chair of the Committee on Graduate Students Department of Electrical Engineering and Computer Science KERR ELECTRO-OPTIC MEASUREMENTS IN LIQUID DIELECTRICS by Xuewei Zhang Thesis Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy Abstract Kerr electro-optic technique has been used to measure the electric field distribution in high voltage stressed dielectric liquids, where the difference between refractive indices for light polarized parallel and perpendicular to the local electric field is a function of the electric field intensity. For transformer oil, the most widely-used insulating liquids in power apparatus and high voltage technology, Kerr effect is very weak due to its low Kerr constant. Previous Kerr measurements have been using ac modulation technique, which is only applicable to dc steadystate electric field mapping while various instabilities develop in liquid under long-term high voltage application. The use of the high-sensitivity CCD camera as optical detector makes it possible to capture the weak Kerr effect in high voltage stressed transformer oil. The first part of this thesis is to demonstrate the reliability and evaluate the sensitivity of the measurements for various cases with identical electrodes under pulsed excitation with insignificant flow effects. After the validation and optimization of the experimental setup, measurements are taken to record the time evolution of electric field distributions in transformer oil stressed by high voltage pulses, from which the dynamics of space charge development can be obtained. Correlation between space charge distribution pattern and impulse breakdown voltage is examined. Hypothetically, bipolar homo-charge injection with reduced electric field at both electrodes may allow higher voltage operation without insulation failure, since electrical breakdown usually initiates at the electrode-dielectric interfaces. It is shown that the hypothesis is testable and correct only under specific circumstances. Besides, fractal-like kinetics for electrode charge injection is identified from the measurement data, which enriches the knowledge on ionic conduction in liquids by offering an experimentally-determined boundary condition to the numerical model. Physical mechanisms based on formative steps of adsorptioni reaction-desorption reveal possible connections between geometrical characteristics of electrode surfaces and fractal-like kinetics of charge injection. The second part of this thesis focuses on the fluctuations in the detected light intensity in Kerr measurements. Up to now, within an experimentally-determined valid range of high voltage pulse duration, the strategy to reduce fluctuation has been taking multiple measurements and then averaging the results. For very short impulses, it is found that the light intensities near the rough surfaces of electrodes both fluctuate in repeated measurements and vary spatially in a single measurement. The major cause is electrostriction which brings disturbances into optical detection. The calculated spatial variation has a strong nonlinear dependence on the applied voltage, which generates a precursory indicator of the electrical breakdown initiation. This result may have potential applications in non-destructive breakdown test and inclusion detection in dielectric liquids. When the applied voltage is dc or ac, signatures of turbulent electroconvection in transformer oil are identified from the Kerr measurement data. It is found that when the applied dc voltage is high enough, compared with the results in the absence of high voltage, the optical scintillation index and image entropy exhibit substantial enhancement and reduction respectively, which are interpreted as temporal and spatial signatures of turbulence. Under lowfrequency ac high voltages, spectral and correlation analyses also indicate that there exist interacting flow and charge processes in the gap. This also clarifies the meaning of dc steady state and the requirement on ac modulation frequency in Kerr measurements. Thesis Supervisor: Dr. Markus Zahn Title: Thomas and Gerd Perkins Professor of Electrical Engineering ii Acknowledgements I wish to thank my thesis supervisor Professor Markus Zahn, for guiding and helping me through my Ph.D. studies at MIT. Working with him has been a great pleasure and valuable experience in my life. I would also like to express my gratitude to my thesis committee members, Professors Cardinal Warde and Joel Schindall, who made constructive suggestions for optimizing the organization and presentation of the thesis. I wish to thank John Kendall Nowocin who made great contributions to upgrading our experimental setup. I also wish to thank former LEES members Hsin-Fu Huang and Shahriar Khushrushahi for their friendship, and LEES staffs, especially Ms. Dimonika Bray, who have helped me a lot in these years. I wish to thank Siemens Corporation and MIT Energy Initiative for the financial support of the research project. I also appreciate the help from the resourceful and patient people in EECS Graduate Office and MIT Libraries. Their help definitely made things much easier for me. I wish to thank my wife and our families for their unconditional love and true understanding. They have always been there to encourage and support me in what I have done, and they have made many sacrifices for me to finish the thesis. Finally, I wish to thank my little princess, Nancy. You are actually far more inspiring than distracting. iii iv Contents Abstract……………………………………………………………………………………………i Acknowledgements……………………………………………………………….……………...iii List of Figures……………………………………………………………………………………ix List of Tables……………………………………………………………………………………xvii 1 Background, motivation and scope of thesis…………………….……………………………1 Synopsis……………………………………………………………………………….…...1 1.1 Background, motivation and research plan……………………………………………2 1.2 Thesis preview………………………………………………………………….……...9 References………………………………………………………………………………..12 2 Evaluating the reliability and sensitivity of the Kerr electro-optic field mapping measurements with high-voltage pulsed transformer oil…………………………………….13 Synopsis………………………………………………………………………………….13 2.1 Introduction…………………………………………………………………………..14 2.2 Principle of Kerr electro-optic field mapping measurement………………………...18 2.3 Experimental setup…………………………………………………………………..22 2.4 Results and discussions……………………………………………………………....27 References……………………………………………………………………………….37 3 Kerr electro-optic field mapping study of the effect of charge injection on the impulse breakdown strength of transformer oil………………………………………………………39 Synopsis…………………………………………………………………………………39 3.1 Introduction………………………………………………………………………....40 3.2 Optimization of Kerr experimental configurations…………………………………44 v 3.3 Experimental procedure…………………………………………………….………….55 3.4 Results and discussions…………………………………………………………....…62 References………………………………………………………………………………..68 4 Transient charge injection dynamics in high-voltage pulsed transformer oil…………….71 Synopsis…………………………………………………………………………………...71 4.1 Introduction…………………………………………………………………………..72 4.2 Identification of fractal-like charge injection kinetics………………………………..77 4.3 Numerical simulations of drift-diffusion conduction model…………………………86 4.4 Discussions……………………………………………………………………………94 References………………………………………………………………………………..97 5 Electro-optic signal fluctuations as indicator of critical transitions in dielectric liquids…………………………………………………………………………………………..101 Synopsis…………………………………………………………………………………101 5.1 Introduction…………………………………………………………………………102 5.2 Indicators of critical transitions in complex systems……………………………….106 5.3 Electro-optic precursor of breakdown initiation in transformer oil….…………...…112 5.4 Discussions………………………………………………………………………….123 References………………………………………………………………………………128 6 Electro-optic signatures of turbulent electroconvection in dielectric liquids under dc and ac high voltages…………………………………………………………………………………131 Synopsis…………………………………………………………………………………131 6.1 Introduction…………………………………………………………………………132 6.2 Spatiotemporal statistical analysis of Kerr electro-optic signal under dc voltages…134 6.3 Spectral analysis of Kerr electro-optic signal under low-frequency ac voltages……144 6.4 Discussions………………………………………………………………………….149 References………………………………………………………………………………160 vi 7 Concluding remarks………………………………………………………………….……...163 A Physical and chemical parameters of transformer oil……………………………………171 B Approaches to improving breakdown strength in liquids………………………………..173 C Pictures of the Kerr electro-optic measurement system..…………………………………219 D List of publications from thesis research………………………………………………….225 vii viii List of Figures Figure 1.1. Experimental setup for Kerr electro-optic field mapping measurements. The beam diameter of the laser (wavelength 632.8 nm) is 0.5 mm and linearly polarized. The 20× beam expander expands the laser beam to about 10 mm in diameter. The polarizers (P0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. P0 is used to ensure the linear polarization state of the expanded laser beam and to attenuate the laser to avoid saturating the CCD camera. The transmission angles of P and A are perpendicular to each other (crossed polarizers). A quarter-wave plate (Q) is inserted between P and the test cell (pre-semi polariscope) to increase measurement sensitivity. The Andor iXon camera is a megapixel back-illuminated EMCCD with single photon detection capability. The imaging area (8×8 mm2) covers the 2 mm gap (~250 pixels across). 3 Figure 1.2. Physical processes in dielectric liquid stressed by a high voltage pulse (no electrical breakdown). 5 Figure 1.3. Two fundamental assumptions made throughout the thesis. 6 Figure 1.4. The research strategy: (1) separation of signal and noise; (2) limited by budget and time, instead of improving accuracy by reducing noise, we study the possible relations of noise to certain physical processes. 7 Figure 1.5. The organization of Chapters 2-6 in the thesis. 9 Figure 2.1. Coordinate system, optical instruments and definition of angles and vectors in Jones calculus. 18 Figure 2.2. Optical component arrangement for linear polariscope. 19 Figure 2.3. Experimental setup for Kerr electro-optic field mapping measurements. The diameter of the pulsed laser beam (wavelength 532 nm) is 7.6 mm and 98% linearly polarized. The polarizers (P 0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. P0 is used to attenuate the laser to avoid saturating the CCD camera. The transmission angles of P and A are 45°and −45°with respect to the x-axis (crossed polarizers). The CCD camera is a megapixel back-illuminated EMCCD with single photon detection capability. The imaging area (8×8 mm2) covers the 2 mm gap (~250 pixels across). 22 Figure 2.4. Representative waveform of the HV pulse from the Marx generator measured by the 5068:1 capacitive divider. Two triggering pulses are generated by the LabVIEW controller to first trigger the camera and the flashlamp and then after 0.1 ms delay trigger the Q-switch to output the laser pulse. 25 Figure 2.5. The view when looking into the window of the test cell. To measure the fringing field, the laser beam and the camera should move correspondingly. The effective exposure time of the CCD is the laser pulse duration (several nanoseconds). 26 Figure. 2.6. Measurements of uniform field without space charge between two aluminum electrodes in transformer oil. The position of the imaging area is shown in Figure 2.5. (a) The distribution of I1(0), where the dark regions to left and right of the illuminated area are electrodes. The light intensity (counts of electrons at a pixel) is represented by the colormap. (b) The distribution of I1(E) − I1(0) when the instantaneous voltage (Uins) is 16 kV; and the camera is triggered at 0.1 ms. (c) The distribution of I1(E) − I1(0) at Uins=24 kV. 29 Figure 2.7. Ratio of I1(E) − I1(0) and I1(0) from the averaged data and power function (exponent=4) fitting. 30 Figure 2.8. Measured field distributions across the gap corresponding to Uins=24 and 16 kV. 30 Figure. 2.9. Relative errors of the measurement results: the maximum deviation of the measured field from uniform field, and the difference between the instantaneous voltage and the integration of the measured field over the gap. 31 ix Figure 2.10. Measurements of space-charge free fringing field with two stainless steel electrodes in transformer oil. The laser beam is shifted to illuminate the fringing area and the position of the CCD imaging area is adjusted correspondingly. (a) The distribution of I1(0). The profiles of the rounded edges of the electrodes can be seen. The light intensity (counts of electrons at a pixel) is represented by the colormap. (b) The distribution of I1(E) − I1(0) when the instantaneous voltage (Uins) is 24 kV and the camera is triggered at 0.14 ms. 33 Figure 2.11. Measured field distributions along Oy axis indicated in Figure 2.10 corresponding to Uins=24 and 16 kV. The dot-dashed lines are numerical simulation results. 33 Figure 2.12. Dependence of the relative error of the measurement results in the range of 0< y <1.5 mm on Uins. 34 Figure 2.13. Measurements with same-material electrode pairs under HV pulses of both polarities. The position of the imaging area is the same as Figure 2.5. The camera is triggered at 0.7 ms with the instantaneous voltage Uins= ±28 kV. For both polarities, the anode is located at x/d=0, while the cathode is located at x/d=1. 35 Figure 3.1 (from [3-2]). Space charge distortion of the electric field distribution between parallel plate electrodes with spacing d at voltage V so that the average electric field is E0=V/d. Four simplest possible configurations are shown: (a) no space charge; (b) unipolar positive or negative charge; (c) bipolar homocharge; (d) bipolar heterocharge. 40 Figure 3.2. Four polariscope configurations: (a) linear; (b) pre-semi; (c) post-semi; (d) circular. 44 Figure 3.3. Numerical results of the intensity ratio when , and when , and vary from to 45 . Figure 3.4. Numerical results of the intensity ratio 48 vary from to . Figure 3.5. Numerical results as Figure 3.6. Numerical results as , and , Figure 3.7 Numerical results of the intensity ratio when varies from to and varies from , ψ and , 49 rad. to . vary from 49 52 to . ,ψ Figure 3.8 Numerical results of the intensity ratio when rad. Figure 3.9 Numerical results of the intensity ratio as to , , and from to varies from 53 53 . Figure 3.10. Experimental setup for Kerr electro-optic field mapping measurements. 56 Figure 3.11. Detected light fields and the distributions of filter. in the gap with and without the spatial 57 Figure 3.12. Electric field distributions (normalized by U(t)/d) from the measurements with a pair of brass electrodes under 30 kV peak HV impulses of positive polarity. The anode and cathode are at 0 and , respectively. The scattered point plots are the measurement results at 0.3, 0.5, and 0.7 ms. 58 x Figure 3.13. Measurement accuracy (a) and fluctuation level (b) as a function of time when the measurements are taken with aluminum electrodes under 30 kV peak HV impulses. 59 Figure 3.14. Determination of the valid time range for the Kerr electro-optic field mapping measurements. 60 Figure 3.15. Local electric fields at anode and cathode under impulsed with 30 kV peak voltage from to ms for 4 combinations of electrode materials: (a) both brass; (b) both aluminum; (c) aluminum anode and brass cathode; (d) brass anode and aluminum cathode. 65 Figure 4.1. The complexity of electric field determination. Given applied voltage and gap configuration, one has to know the interactions between electric field and space charge to solve for electric field. However, quantitative account of the electrode charge injection is difficult. 72 Figure 4.2. Illustration of the three-step scheme for charge injection: specific adsorption, charge transfer reaction in EDL, desorption. While charge transport is drift-dominated in the bulk of the liquid, the EDL processes injecting charges at the metal-liquid interface are diffusion-limited, which, as will be shown later in this chapter, are closely related to the roughness of electrode surfaces via fractal geometry concepts and models. 74 Figure 4.3. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 10 kV. 78 Figure 4.4. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 20 kV. 78 Figure 4.5. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 30 kV. 79 Figure 4.6. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 10 kV. 79 Figure 4.7. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 20 kV. 80 Figure 4.8. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 30 kV. 80 Figure 4.9. Time evolution of , total injected charge per unit electrode area, plotted in linear coordinates: case (I). 82 Figure 4.10. Time evolution of , total injected charge per unit electrode area, plotted in linear coordinates: case (II). 83 Figure 4.11. Time evolution of , total injected charge per unit electrode area, plotted in log-log coordinates: case (I). The solid lines are the results of linear fitting. 83 Figure 4.12. Time evolution of , total injected charge per unit electrode area, plotted in log-log coordinates: case (II). The solid lines are the results of linear fitting. 84 Figure 4.13. Numerical solutions of electric field distribution under 30 kV applied voltage at 0.25 ms and 0.75 ms. The number of spatial steps is 200; the number of time steps is 2000. (a) Crank-Nicolson; (b) The Crank-Nicolson with implicit Euler for the first 10 time steps. 90 Figure 4.14. Numerical solutions of the local electric fields near anode and cathode surfaces: case (I), anode. 91 xi Figure 4.15. Numerical solutions of the local electric fields near anode and cathode surfaces: case (I), cathode. 91 Figure 4.16. Numerical solutions of the local electric fields near anode and cathode surfaces: case (II), anode. 92 Figure 4.17. Numerical solutions of the local electric fields near anode and cathode surfaces: case (II), cathode. 92 Figure 4.18. Mechanisms for fractal-like charge injection kinetics. (a) If the surface reaction is adsorptionlimited, on rougher surfaces, the protrusions are dominant in adsorbing neutral molecules (D is the diffusion constant, t is the duration of HV pulses), while on smoother surfaces, the pores also make significant contributions. (b) If the surface reaction rate is controlled by lateral diffusion of reacting molecules, anomalous diffusion along fractal surface may account for the origin of fractal charge injection kinetics. 95 Figure 5.1. Typical voltage (a) and corresponding current (b) waveforms when a pair of stainless steel electrodes are stressed by 1 µs/1 ms high voltage pulses. 107 Figure 5.2. (a) Bifurcation diagram of a model desert vegetation system undergoing predictable sequence of spatial patterns as approaching a critical transition (from [5-23], which was modified from [5-29]). (b) The breakdown probability as a “function” of applied voltage. Catastrophic bifurcation may or may not exist. In either case small forcing (i.e. increase in voltage) will lead to a distinct state. 109 Figure 5.3. (a) The image of the gap illuminated by an expanded laser beam. (b) The background light intensity distribution in the gap leaked from crossed polarizers as the 1 mm gap is illuminated by a Gaussian beam (7.6 mm in diameter). The region of interest (ROI) is recorded in a 120-by-60 (row-by-column) matrix. 113 Figure 5.4. The distributions of fluctuations (normalized by the averages) of the measured pixel light intensities in multiple measurements. (a) with no high voltage pulse generated, at most pixels, the standard deviations of the light intensities in the 1,000 measurements stay below 5% of the averaged light intensities; (b) with high voltage pulses firing nearby, there is no substantial difference in the fluctuation level compared with (a), indicating that electromagnetic compatibility is adequate for our measurement system. 114 Figure 5.5. (a) Same as Figure 5.4(a). With no applied voltage, the standard deviations of the light intensities at most pixels in the 1,000 measurements stay around 5% of the averaged light intensities. (b) The histograms and fitted normal distributions of the light intensities at two pixels, #1 and #2 marked in (a). 115 Figure 5.6. The average fluctuations in row i=1(cathode), 60(mid-gap), and 120(anode) at various stantaneous voltages with rise-time of the pulses being (a) 100 µs, (b) 1 µs, and (c) 10 ns. (d) is an illustration of matrix , which is used to store the pixel light intensity distribution in the ROI. 117 Figure 5.7. For 3 cases with about the same instantaneous voltage (+30 kV) but different rise times from 10 ns to 100 µs, the distributions of average fluctuations across the gap are shown, and the pixels with strongest fluctuations (>10%) are marked. 119 Figure 5.8. The slice-by-slice image entropy distributions with zero and 30 kV applied voltages. 120 Figure 5.9. The coefficient of spatial variance of the cathode slice as a function of applied voltage. The error bars are drawn based on the data from multiple measurements. 121 Figure 5.10. A phenomenon similar to critical slowing down. (a) The 1 ms square wave pulse and the ratio of the detected light intensity and the zero field value. All light intensities have been averaged over the ROI. (b) For 10, 20, 30 kV pulses, the time it takes for the light intensity to drop to the zero field value is approximately 1, 3, 10 ms, respectively. 124 Figure 5.11. (From [5-32]) Localized discharges (streamers) on cathode on uniform electric field. The gap spacing is 4 mm. The liquid is n-hexane. The image was taken about 1 µs before breakdown. 125 xii Figure 5.12. (From [5-9], page 17) Experiment on electrostriction wave excitation in water in the system of extended electrodes (slit scanning). 126 Figure 6.1. The view as looking into the window of the test cell. The diameter of the pulsed laser beam is 7.6 mm. The imaging area (8×8 mm2) of the CCD camera has an array of 1002×1004 pixels. The width of the gap between two parallel-plate electrodes is d=2 mm, corresponding to about 250 pixels. The 1×1 mm2 region of interest (ROI) is chosen around the center of the gap. 135 Figure 6.2. Histogram (bar plot, 500 samples, 5 Hz sampling rate), normal fitting (solid line), and lognormal fitting (dashed line) of the distribution of detected light intensities without high voltage (HV) application. The inset shows the light intensity fluctuations in time. 135 Figure 6.3. The skewness of the detected light intensity distribution as a function of applied HV. The error bars come from statistics at various pixels in ROI. The three regions partitioned by the two dashed lines indicate that the data is very likely skewed positively (above), negatively (below), and inconclusively (middle). The two insets of histograms of light intensities show the slightly (8 kV) and strongly (18 kV) positively-skewed distributions. 136 Figure 6.4. The dependence of scintillation index (S) and conduction current on applied HV. 138 Figure 6.5. ROI image entropy (normalized by H0, the value in the absence of HV) versus applied HV under 3 different experimental conditions. 140 Figure 6.6. The scintillation index S evaluated with L-by-L binning (i.e., the statistics is based on the average light intensity in a square region containing L× L pixels). The dashed line indicates the scintillation level corresponding to about 10% detection uncertainty. The applied HV is 20 kV. 141 Figure 6.7. Results of Kerr electro-optic field mapping measurements under 2 different experimental conditions, both of which are heterocharge configuration with enhanced electric fields near the electrodes. The applied HV is 20 kV. 142 Figure 6.8. The scintillation index S evaluated with various exposure times. The dashed line indicates the scintillation level corresponding to about 10% detection uncertainty. The applied HV is 20 kV. 142 Figure 6.9. Detected light intensities at two pixels labeled 1 and 2 (100 pixels or 0.8 mm apart) when the applied HV is sinusoidal with amplitude 20 kV and frequency fac=0.1 Hz. The sampling rate is 63.53 Hz. A sample image is presented in the inset, in which the bright band actually bounces between the two electrodes at frequency fac. 144 Figure 6.10. Fourier spectra magnitude versus frequency at pixels 1 and 2. The dashed lines are the spectra in the absence of HV. 145 Figure 6.11. The coefficient of correlation between the time series of light intensities at pixels 1 and 2 (2’, which is 10 pixels away from 1) as a function of applied HV amplitude. 147 Figure 6.12. Fourier spectra magnitude versus frequency at pixel 1 with HV amplitude 20 kV and 3 different fac values. The sampling rate is 80 Hz. Figure 6.13. Illustration of experimental setup for Kerr electro-optic field mapping measurements with ac modulation. 147 Figure 6.14. Errors in measured dc and ac electric fields with dc voltage (d) kV and various modulation voltages ( ) and frequencies ( ). kV; 154 Figure 6.15. Reasonable ranges of ac modulation frequencies and amplitudes for 5 kV, 10 kV and 18 kV. For each , the reasonable range is the set of the parameter pairs at the same side of the corresponding curve as the arrow. 156 xiii (a) kV; (b) kV; (c) 150 Figure 6.16. Normalized dc electric field distribution between copper electrodes in transformer oil under various dc voltages ( ) measured with ac modulation 10 kHz and 0.5 kV. 158 Figure B.1 (from Ref. [6]). Dependence of breakdown strength Ebd (MV/cm) on time τ (μs) in saturated hydrocarbons with gap separation of 63.5 μm: a, hexane; b. heptane; c, octane; d, nonane. 184 Figure B.2 (from Ref. [6]). Dependence of breakdown strength Ebd (MV/cm) on liquid density ρ (g/cm3) under various experimental conditions: a, normal paraffin, τ = 1.4 μs; b, single branched-chain hydrovarbons, τ = 1.4 μs; c, double branched-chain hydrocarbons, τ = 1.4 μs; d, normal paraffin, direct voltage; e, single branched-chain hydrocarbon, direct voltage; f&g, straight and branched-chain benzene derivatives, τ = 1.65 μs; h, silicons, dc. 185 Figure B.3 (from Ref. [6]). Dependence of breakdown voltage Vbd (kV) on electrode separation δ (μm) for a number of electrode materials and cathode shapes: flat cathode: a, Cr; b, Cu; c, Al (flat cathode); d, Cr, Cu, Al (point cathode). 185 Figure B.4 (from Ref. [6]). Dependence of breakdown strength Ebd (kV/cm) on the number of breakdowns N in transformer oil. The dashed lines indicate the limits of scatter of experimental results. 186 Figure B.5 (from Ref. [8]). Voltage-time characteristics of a transformer oil with tip-plane gap configuration for d = 5 (1), 15 (2), and 25 cm (3). 195 Figure B.6 (from Ref. [8]). Dependence of breakdown voltage of perfluorohaxane on the frequency in the tipplane gap for an inter-electrode distance of 1.9mm. 196 Figure B.7 (from Ref. [8]). Dependence of the electric strength of the NaCl aqueous solution on the electrical conduction in a uniform field at td = 70 ns and d = 0.02 cm (a) and in a non-uniform field at td = 90 ns and d = 0.015 cm (b) for −T +P (curve 1) and +T −P electrodes (curve 2). 198 Figure B.8 (from Ref. [8]). Dependences of the relative electric field strength (a) and standard deviation of the water breakdown field strength (b) as function of the β-alanine concentration for austenite (curve 1), ferrite stainless steel (curve 2) and aluminum electrodes (curve 3). 200 Figure B.9 (from Ref. [12]). Breakdown electric field as a function of distance between electrodes with (a) different material pairs and (b) different impurity concentrations. 202 Figure B.10 (from Ref. [20]). (a) Scheme of the test cell; (b) 50% lightning impulse breakdown voltage vs. relative position (a1/a) of the barrier for a=50 mm. 204 Figure B.11 (from Ref. [23]). Influence of testing procedures on the breakdown behavior of in- 205 service contaminated oil. Figure B.12 (from Ref. [26]). (a) Typical dielectric strength course of insulators in insulation systems; (b) long term degradation in ac liquid breakdown strength. Figure B.13 (from Ref. [31]). Resistivity as a function of water content in (a) benzene and (b) toluene. 207 Figure B.14 (from Ref. [37]). Breakdown voltage evolution of oils and mixtures with 6 measurements. [Water content (ppm) / Pollution class (NAS 1638)]. 211 Figure C.1. Small Kerr cell with optical components. 219 Figure C.2. Large Kerr cell with utility grade capacitor used for substation power factor correction. 222 xiv 208 Figure C.3. Electrode holder (beginning design) and electrode module (final design). 222 Figure C.4. Filter canister (3 µm filter rating) and variable speed gear pump drive for oil filtering and circulation. 223 xv xvi List of Tables Table 3.1. Numerical results of as , and Table 3.2. Numerical results as in the range of , and has a deviation of 46 . . 47 Table 3.3. Impulse breakdown test results for combinations of brass and aluminum electrodes under both polarities. 62 Table 3.4. Impulse breakdown test results for combinations of brass and stainless steel (S-S) electrodes. 67 Table A.1. Physical and chemical parameters of the transformer oil. 171 Table B.1. Dependence of electrical breakdown strength of insulating liquids on various factors (extracted from Ref. [7]). 190 Table B.2. Effect of polarity on breakdown initiated in various liquids for a tip-plane electrode system at T = 293 K (From Ref. [8]). 196 Table B.3. Comparing withstand voltages of non-parametric and parametric methods (from Ref. 212 [41]). xvii xviii 1 Background, motivation and scope of thesis Synopsis This thesis focuses on Kerr electro-optic measurements in transformer oil. At first glance, there seems to be nothing attractive in this research: old physics (Kerr effect was discovered over 100 years ago and molecular theory of Kerr effect was established over 50 years ago), mature technique (Kerr electro-optic field mapping in liquids was extensively studied in the 1960s80s), and traditional material (transformer oil is the most widely-used insulating liquid in industry). In this introductory chapter, it will be shown that there still exist new grounds to break. Section 1.1 presents background, motivation, and plan (including fundamental assumptions and research strategies) of the thesis. Section 1.2 discusses the structure of the thesis and gives a preview of each subsequent chapter. 1 1.1 Background, motivation and research plan The dielectric liquid used in the thesis research is transformer oil (important physical and chemical parameters are listed in Appendix A). Transformer oil is the most widely used dielectric liquid for high voltage insulation and power apparatus cooling due to its greater electrical breakdown strength and thermal conductivity than gaseous insulators and its ability to self-heal and conform to complex geometries that solid insulators do not have [1-1]. The insulating properties of transformer oil have been extensively studied in attempt to understand the basic mechanisms of electrical breakdown [1-2] and to prevent the disastrous consequences of insulation failure [1-3]. To improve the electrical breakdown strength (a comprehensive literature review on this topic is provided in Appendix B), it would be necessary to know the electric field distribution in an insulation configuration, which, however, cannot be directly calculated from information on electrode configuration, dielectric properties and source excitation. Space charge originating from bulk dissociation in high voltage stressed oil and charge injection by high voltage stressed electrodes can significantly distort the electric field distribution and play an important role in the insulation failure [1-4]. Theoretically, this formulates a highly nonlinear problem in which the generation and motion of space charge are determined by the electric field; and meanwhile space charges have a ‘feedback’ on the latter according to Gauss’ law. To numerically simulate the physical processes, the main difficulty lies with the quantification of electrode charge injection as a function of dielectric and electrode materials, impurity contents, electrode surface condition, etc. More experimental data are needed to test the assumptions in some analytical models or propose any new theory. 2 Figure 1.1. Experimental setup for Kerr electro-optic field mapping measurements. The beam diameter of the laser (wavelength 632.8 nm) is 0.5 mm and linearly polarized. The 20× beam expander expands the laser beam to about 10 mm in diameter. The polarizers (P0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. P0 is used to ensure the linear polarization state of the expanded laser beam and to attenuate the laser to avoid saturating the CCD camera. The transmission angles of P and A are perpendicular to each other (crossed polarizers). A quarter-wave plate (Q) is inserted between P and the test cell (pre-semi polariscope) to increase measurement sensitivity. The Andor iXon camera is a megapixel back-illuminated EMCCD with single photon detection capability. The imaging area (8×8 mm2) covers the 2 mm gap (~250 pixels across). High voltage stressed liquids are usually birefringent, in which case the refractive indices for light (of free-space wavelength ) polarized parallel ( ) and perpendicular ( the local electric field are related by , where is the Kerr constant and ) to is the magnitude of the applied electric field. In parallel-plate electrode configuration, we assume the magnitude and direction of to be constant along the light path. Thus the phase shift between light-field components polarized parallel and perpendicular to the applied electric field and propagating along electrode length is . The modulation effect of the electric field can be detected by comparing the intensities of incident light and transmitted light. 3 In this thesis, the Kerr electro-optic approach will be used to measure the electric field distributions between parallel-plate electrodes in transformer oil. One of the experimental setups for the Kerr electro-optic field mapping measurements is illustrated in Figure 1.1 (in Appendix C, some photos of the experimental setup are provided). Previous works [1-5, 1-6] mainly deal with high Kerr constant materials like propylene carbonate ( ( m/V2). For small Kerr constant material like transformer oil m/V2), to improve the detection sensitivity, ac modulation method [1-7, 1-8] has proven to be effective in dc ‘steady state’ measurements. The steady state in quotation implies that in reality there may not be one due to the induced flow as the dc high voltage keeps on. On the other hand, the principles of ac modulation do not work for short high voltage pulses ( ms) with insignificant flow effects, since the lock-in amplifier used in this method needs at least several seconds to register a signal. Kerr measurements in high voltage pulsed low Kerr constant transformer oil without ac modulation thus presents a challenge in this research area. We summarize the possibly new grounds to break as follows: Firstly, many aspects of transformer oil have been intensively studied. However, there remains a lack of detailed accounts of various physical processes of transformer oil stressed by high electric field. Models proposed make various assumptions and approximations which might be unrealistic. Secondly, most of the previous Kerr measurements were taken for liquids with Kerr constants 2-3 orders higher than that of transformer oil. For transformer oil, a technique called ac modulation method was developed. But the drawback of ac modulation is that it assumes the existence of steady state which would be invalid in strong electric fields. In this sense, the measurement technique for transformer oil is not mature at all. 4 Finally, the measurable Kerr effect in transformer oil is always mixed with other physical effects such as electrostrictive shock wave, charge injection and transport, and electrohydrodynamic (EHD) turbulence. New physics may lie with a careful separation of these effects. The central question that is set out to answer in the thesis is: what information on the underlying physical processes can be extracted from the data of Kerr measurements with transformer oil? To be more specific, there are different aspects of this question. Under what conditions can the electro-optic signals be used to map electric field distribution? How to ensure the accuracy and reliability of the measurement data? What are the sources of noise and uncertainties in the measurement system? Are they random, biased, or patterned? Before outlining the experimental work, the fundamental assumptions made throughout the thesis are to be introduced. Conceptually, the thesis is based on the understanding of basic physical processes in dielectric liquid stressed by a high voltage pulse (no electrical breakdown) shown in Figure 1.2. To take valid field mapping measurements, the experimental systems should be able to separate the time scales shown in Figure 1.2. Electrostrictive Shock Wave Ionic Conduction Processes (Time range: ~ rise time of the pulse) (Electrode injection, charge generation, recombination, drift, diffusion, etc.) Charge Migration Time (EHD enhanced conduction) Electrohydrodynamic HV Pulse convection Duration Viscous Diffusion Time Figure 1.2. Physical processes in dielectric liquid stressed by a high voltage pulse (no electrical breakdown). 5 Depending on the high voltage duration, there are three types of physical processes: electrostriction (caused by the sudden change of electric field which establishes pressure gradients; the relaxation and dissipation of this shock wave behavior are very rapid); ionic conduction which bring in space charge processes (the characteristic time for this process is called charge migration time, i.e. the time it takes for a charge carrier to transport over a distance, the evaluation of which can be found in Chapter 2); electroconvection (a short term for EHD convection due to Coulomb force on charges in the liquid, the onset of which is usually evaluated by the viscous diffusion time; see Chapter 3 for details). Kerr Constant Assumption 1: The Kerr constant of the dielectric liquid for light wave of a given frequency is the same in the 1~10 kV/mm electric field range. 1 10 Electric Field (kV/mm) (a) ~d Assumption 2: The effective range of fringe field is about the width of the inter-electrode gap, d; the electro-optic modulation in the fringe area can be neglected if the length of electrodes is much larger than d. Electrode d Light Propagation Electric Field Electrode (b) Figure 1.3. Two fundamental assumptions made throughout the thesis. 6 On the technical side, there are two fundamental assumptions made as illustrated in Figure 1.3. The first is that for light wave of a given frequency, the Kerr constant of the dielectric liquid is the same in the electric field range of our measurements (1~10 kV/mm), which means that the Kerr constant depends only on the liquid, e.g. the molecular structure, permittivity, etc. Although no independent measurements were designed to test this assumption (mainly because the electric field becomes distorted in an unknown way as the voltage gets higher), the field mapping results (Chapter 2 and Chapter 3) with adequate accuracy will verify this assumption to some extent. The second assumption is that the fringe field effect is neglected. The light wave front may get distorted due to the inhomogeneous anisotropic nature of this part of the media. In our treatment, the effective range of fringe field is about the width of the inter-electrode gap, d; the electro-optic modulation in the fringe area tends to be negligible if the length of electrodes is much larger than d. In principle, numerical methods such as wave-propagating and ray-tracing can be used to estimate fringe field effect. However, this is out of scope of the thesis. Validation of Experimental Approach Signal Electric field and space charge Noise Relation to specific physical process Improve measurement accuracy Figure 1.4. The research strategy: (1) separation of signal and noise; (2) limited by budget and time, instead of improving accuracy by reducing noise, we study the possible relations of noise to certain physical processes. 7 To achieve the research goal, new instruments and new insights play equally important roles. A high-sensitivity high-resolution CCD is used to detect the Kerr effect without ac modulation, thus making transient measurements possible. The first challenge along the way is that the CCD can register a considerable amount of noise, even if everything has been done to make the experimental system as precise as possible. It is natural to think of taking multiple measurements and then averaging the results. As illustrated in Figure 1.4, after the reliability and accuracy of this method has been evaluated and confirmed, we study signal (average) and noise (fluctuation) separately. The former is the traditional field mapping measurements with much higher sensitivity thanks to our CCD camera. Measurements of transient electrical conduction dynamics in transformer oil under high voltage impulses are taken. Correlation between charge injection pattern and impulse breakdown voltage is also an interesting topic. The latter was supposed to focus on the identification of various noise sources and methods to reduce the negative effects of noise. However, due to the limited budget and time, we were not able to purchase better measurement instruments for an upgraded experimental system. Since the noise level in the measurement results seems unlikely to improve significantly in the current settings, we study the “message” in the noise, i.e. the fluctuations in the detected light intensities, and explore the possible relations of noise to specific physical processes that are the major contributors to it. As we will see in Chapter 5 and Chapter 6, this compromise in fact led to some interesting findings. 8 1.2 Thesis preview The schematic in Figure 1.5 shows the organization of 5 core chapters of the thesis. Chapter 2 is the foundation of other chapters since it presents the validation of the experimental approach. Chapter 3 and Chapter 5 discuss topics related to electrical breakdown (this is why they are placed at the higher electric field positions). Chapter 4 and Chapter 6 discuss conduction with and without electrohydrodynamic processes; the electric field is much HV Electric Field lower than the breakdown strength). Chapter 5 Chapter 3 Electrostriction-induced noise ↕ Impulse breakdown initiation Charge injection pattern ↕ Impulse breakdown voltage Chapter 2: Validation Electroconvection-related noise Transient charge injection dynamics Chapter 4 Chapter 6 HV Pulse Duration Figure 1.5. The organization of Chapters 2-6 in the thesis. An alternative perspective to view the organization of the chapters is based on the physical processes shown in Figure 1.2. Chapter 2, Chapter 3, and Chapter 4 are all on conduction processes (field mapping based on the averaged signal), while Chapter 5 and Chapter 6 are on noise related to electrostriction (short impulse) and electroconvection (longer pulse, dc or ac voltages). The contents of subsequent chapters are described as follows: 9 In Chapter 2, with the help of a high-sensitivity charge-coupled device (CCD), the Kerr electro-optic effect is directly measured between parallel electrodes in transformer oil stressed by high voltage pulses. In this chapter, we demonstrate the reliability and evaluate the sensitivity of the measurements for three cases with identical electrodes: space-charge free, uniform electric field in the mid-region of the gap; space-charge free, non-uniform fringing electric field; and space charge distorted electric field in the mid-region of the gap. Different criteria are used to determine the measurement accuracy. Future directions to improve accuracy by identifying and handling various sources of error and noise are suggested. The smart use of charge injection to improve breakdown strength in transformer oil is demonstrated in Chapter 3. Hypothetically, bipolar homo-charge injection with reduced electric field at both electrodes may allow higher voltage operation without insulation failure, since electrical breakdown usually initiates at the electrode-dielectric interfaces. To find experimental evidence, the applicability and limitation of the hypothesis is first analyzed. Impulse breakdown tests and Kerr electro-optic field mapping measurements are then conducted with different combinations of parallel-plate aluminum and brass electrodes stressed by millisecond duration impulse. It is found that the breakdown voltage of brass anode and aluminum cathode is ~50% higher than that of aluminum anode and brass cathode. This can be explained by charge injection patterns from Kerr measurements under a lower voltage, where aluminum and brass electrodes inject negative and positive charges, respectively. In Chapter 4, transient electrode charge injection in high-voltage pulsed transformer oil is studied with Kerr electro-optic measurements. Time evolutions of total injected charges and injection current densities from two stainless-steel electrodes with distinct surface roughness obey a power law with different exponents. Numerical simulation results of the time-dependent 10 drift-diffusion model with the experimentally-determined injection current boundary conditions agree with measurement data. The power-law dependence implies that the electric double layer processes contributing to charge injection are diffusion-limited. Possible mechanisms are proposed based on formative steps of adsorption-reaction-desorption, revealing deep connection between geometrical characteristics of electrode surfaces and fractal-like kinetics of charge injection. In Chapter 5, motivated by the search for approaches to non-destructive breakdown test and inclusion detection in dielectric liquids, we explore the possibility of early warning of breakdown initiation in high voltage pulsed transformer oil from the data of Kerr electro-optic measurements. It is found that the light intensities near the rough surfaces of electrodes both fluctuate in repeated measurements and vary spatially in a single measurement. We show that the major cause is electrostriction which brings disturbances into optical detection. The calculated spatial variation has a strong nonlinear dependence on the applied voltage, which generates a precursory indicator of the critical transitions. Signatures of turbulent electroconvection in transformer oil stressed by dc and ac voltages are identified from Kerr electro-optic measurement data in Chapter 6. It is found that when the applied dc voltage is high enough, compared with the results in the absence of high voltage, the optical scintillation index and image entropy exhibit substantial enhancement and reduction respectively, which are interpreted as temporal and spatial signatures of turbulence. Under low-frequency ac high voltages, spectral and correlation analyses also indicate that there exist interacting flow or charge processes in the gap. This chapter also clarifies some fundamental issues on Kerr measurements. 11 References [1-1] R. Bartnikas (ed.), Engineering Dielectrics: Electrical Insulating Liquids, Vol. 3 (ASTM, Philadelphia, 1994). [1-2] I. Adamczewski, Ionization, Conductivity and Breakdown in Dielectric Liquids (Taylor&Francis, London, 1969). [1-3] V. Y. Ushakov, Insulation of High-Voltage Equipment (Springer-Verlag, Berlin, 2004). [1-4] M. Zahn, “Optical, Electrical and Electromechanical Measurement Methodologies of Field, Charge and Polarization in Dielectrics”, IEEE Trans. Dielectr. Electr. Insul. 5, 627 (1998). [1-5] E. C. Cassidy, H. N. Cones, and S. R. Booker, “Development and Evaluation of ElectroOptic High-Voltage Pulse Measurement Techniques”, IEEE Trans. Instr. Meas. 19, 395 (1970). [1-6] A. Helgeson and M. Zahn, “Kerr Electro-Optic Measurements of Space Charge Effects in HV Pulsed Propylene Carbonate”, IEEE Trans. Dielectr. Electr. Insul. 9, 838 (2002). [1-7] A. Törne and U. Gäfvert, “Measurement of the Electric Field in Transformer Oil Using Kerr Technique with Optical and Electrical Modulation,” in Proceedings, ICPADM, Vol. 1, Xi’an China, 24-29 June 1985, pp. 61-64. [1-8] T. Maeno and T. Takada, “Electric Field Measurement in Liquid Dielectrics Using a Combination of ac Voltage Modulation and a Small Retardation Angle”, IEEE Trans. Electr. Insul. 22, 503 (1987). 12 2 Evaluating the reliability and sensitivity of the Kerr electro-optic field mapping measurements with highvoltage pulsed transformer oil Synopsis Transformer oil is the most widely used dielectric liquid for high voltage (HV) insulation. Measurements of the electric field distribution in high voltage pulsed transformer oil are of both practical and theoretical interests. Due to its low Kerr constant, previous electro-optic measurements with transformer oil rely on a technique called ac modulation, which is primarily used only for dc steady-state electric field mapping. With the help of a high-sensitivity chargecoupled device (CCD), the Kerr electro-optic effect is directly measured between parallel electrodes in transformer oil stressed by high voltage pulses. In this chapter, we demonstrate the reliability and evaluate the sensitivity of the measurements for three cases with identical electrodes: space-charge free, uniform electric field in the mid-region of the gap; space-charge free, non-uniform fringing electric field; and space charge distorted electric field in the midregion of the gap. Different criteria are used to determine the measurement accuracy. Future directions to improve accuracy by identifying and handling various sources of error and noise are suggested. 13 2.1 Introduction As mentioned in Chapter 1, transformer oil is the most widely-used dielectric liquid for high voltage (HV) insulation. To improve the electrical breakdown strength, it is necessary to know the electric field distribution in an insulation configuration. Due to the space charge effect, generally the electric field distribution cannot be calculated from the information of electrode configuration, dielectric properties and source excitation alone. A comprehensive description of the mechanisms and mathematical models of space charge generation and motion will be given in Chapter 4. Here we only briefly introduce the basic physical picture. In addition to dielectric liquid ionization and flow electrification, electrode charge injection is thought to be a primary cause of space charge generation [2-1]. The electrode injection includes two well-conceptualized charge transfer processes at the electrode-dielectric interfaces [2-2]: emission and capture of electrons by the metal electrodes, and equilibrium or non-equilibrium electric double layer dynamics. Contaminants (e.g. bubbles and/or particles adhered to the surfaces and suspended in the liquid) and chemical/electrochemical reactions between the electrode material and the liquid (e.g. specific adsorption) all contribute to charge injection [2-3]. For practical liquid dielectrics like transformer oil, it remains challenging to disentangle the complexity and characterize it quantitatively. Partly it is because the molecular structure and chemical composition of the oil (containing at least tens of different compounds, with various impurities and contaminants) are not as simple and regular as those of gases or solids, which makes systematic investigation of its electrical behavior on microscopic scale extremely 14 difficult and sometimes inconsistent. Theoretically, the bipolar ionic drift-diffusion model has been formulated to analyze dc steady-state conduction [2-4] and transient behavior under a step excitation [2-5], in which electrode charge injection is included as a boundary condition, i.e. specified charge densities at the electrode-liquid interfaces. However, in strong dc field conduction, the thermohydrodynamic and electro-hydrodynamic effects are significant [2-6] in liquids. The former is caused by a temperature/pressure gradient induced by electrical current/stress, while the latter is the motion due to the Coulomb force on space charge in the fluid. Therefore, the model seems more appropriate for describing the response under a short HV pulse. As a prerequisite for the verification and improvement of the theoretical model, reliable and accurate measurement data on the electric field distribution and its dynamics under pulsed HV is needed. The Kerr electro-optic technique [2-7] has been used to measure the electric field distribution in HV stressed liquids, where the refractive indices for light (with free-space wavelength ) polarized parallel, related by , and perpendicular, ( is the Kerr constant and , to the local electric field are is the electric field intensity). In a parallel-plate electrode geometry, the -field vector is assumed to be constant along the light path. Thus, after propagating through the electrode length , the phase shift components polarized parallel and perpendicular to the field is between light , which can be measured with two crossed or aligned polarizers. In Section 2.2, we will present a more detailed introduction to the Kerr electro-optic effect and its measurement. For low Kerr constant transformer oil ( traditional approach to make ~ m/V2), is very small, and the detectable in dc steady-state measurements is using an 15 indirect method [2-8], in which an ac modulation voltage (frequency f is so high that the ac field has negligible effect on space charge behavior) is superposed to the dc HV. The total electric field E has both dc and ac components. The phase shift , proportional to E2, will correspondingly have a dc component and two ac components with frequencies f and 2f (although very weak, the ac components can be measured by lock-in amplifiers), from which the dc electric field can be calculated (this method will be demonstrated in Chapter 6). The limitations of the ac modulation method are two-fold: (a) in reality there may not be a dc steady state due to the induced flow under higher voltages; (b) it does not work for short HV pulses (e.g. ~10 ms in duration) with insignificant flow effects, because it takes at least seconds for the lock-in amplifier to register stable ac components. For this reason, taking Kerr measurements in HV pulsed transformer oil without ac modulation has been considered as a challenge in this research area. Meanwhile, if it is realized, our understanding of the conduction and breakdown mechanisms in transformer oil will be greatly enriched. In this thesis, with the help of a high-sensitivity charge-coupled device (CCD), Kerr electro-optic field mapping measurements are conducted to determine the electric field distribution between parallel electrodes in transformer oil stressed by HV pulses. The CCD camera with single photon detection capability is used to measure the light intensity of a pulsed laser beam coming through the Kerr test cell (we will also use an intensity-stabilized continuous wave laser in Chapter 3). High sensitivity is a double-edged sword. It makes possible the direct detection of the small modulation effects in transformer oil. However, along with the signal of the Kerr effect, noise originating from various uncertain and random processes in the system is also recorded. 16 For example, even without HV, the shot-to-shot variation of the light intensity at one pixel (8×8 µm2) can be as high as 20% (averaging the data from multiple measurements can lower this noise level to ~5%). This is because on the one hand the laser output has intrinsic spatiotemporal fluctuations, and on the other hand the laser beam propagates in a medium with randomness (scattering, turbulence, etc). Due to the presence of noise, the major concerns of this chapter are the reliability and accuracy of the Kerr electro-optic field mapping measurements, which will be evaluated from the following three aspects: (1) measurements of space-charge-free, uniform field in the middle section of the gap; (2) measurements of space-charge-free, non-uniform fringing field; and (3) measurements of space charge distorted field in the middle section of the gap between samematerial electrodes. The estimation of the accuracy and sensitivity will be made by comparing the measurement results of the space-charge-free fields with theoretical predictions. The organization of the rest of this chapter is as follows: in Section 2.2, we will describe the principles of field mapping measurements based on the Kerr electro-optic effect; an introduction to the experimental setup and instrumentation for our measurements will be given in Section 2.3; finally, after defining two criteria of the measurement accuracy, data from measurements will be analyzed. It will be shown that Kerr measurements can produce physically reasonable and self-consistent results in all the three cases above. 17 2.2 Principle of Kerr electro-optic field mapping measurements In general, all materials exhibit the Kerr effect, or electric field induced birefringence, but it is dominant only for centrosymmetrical materials such as liquids or glasses. Dielectric liquids, which in natural state are isotropic due to random molecular orientation, become birefringent when stressed by electric fields. The refractive indices for light (with free-space wavelength ) polarized parallel, related by , and perpendicular, ( is the Kerr constant and , to the local electric field are is the electric field intensity). In a parallel-plate electrode geometry, the -field vector is assumed to be constant along the light path. Thus, after propagating through the electrode length , the phase shift between light components polarized parallel and perpendicular to the field is . Next we will use the Jones matrix [2-9] representation of light propagation through optical elements as a concise method to obtain the relation between the initial and final light intensities in Kerr electro-optical experiments. x ein x y z Polarizer (analyzer) x Transmission axis y Laser eout y z Detector Birefringent components x Slow axis y Figure 2.1. Coordinate system, optical instruments and definition of angles and vectors in Jones calculus. As shown in Figure 2.1, the light propagation is along the z-axis, and the vectors of both the light electric field (optical polarization) and the applied HV field (dielectric polarization) 18 are in the x-y plane transverse to light propagation. Note that in Jones calculus, the light field vector is represented by complex amplitude e, i.e. the actual light field is the real part of , where , is the time, and is the (angular) frequency of the light. For polarizer (or analyzer), supposing the transmission axis is at angle θ with respect to the y-axis, the Jones matrix is defined by: exout cos out e sin y sin 2 sin cos sin 0 0 cos cos 0 1 sin sin exin cos einy (2.1) in ein sin cos ex in U p ( ) xin e cos 2 e y y For birefringent components like a quarter-wave plate and the Kerr cell, supposing the slow axis is at angle ψ with respect to the y-axis and the slow wave is retarded by Δφ in phase, we have: exout cos out e sin y sin 1 0 cos i cos 0 e sin sin exin cos einy (2.2) ein cos 2 e i sin 2 cos sin (e i 1) exin in U b ( , ) xin i e 1) sin 2 e i cos 2 ey cos sin (e y For a quarter-wave plate, in Equation (2.2). For a Kerr cell, , and the slow axis is along the direction of applied HV field. Polarizer Grounded electrode E y e0 Laser beam Kerr medium x Analyzer y High-voltage electrode z e1 x z Figure 2.2. Optical component arrangement for linear polariscope. 19 Figure 2.2 is a linear polariscope (without quarter-wave plates), the simplest combination of basic Jones matrices defined in Equations (2.1)&(2.2). For the configuration shown in Figure 2.2, supposing the complex amplitude of the electric field of the linearlypolarized light is e0 at the laser side and e1 at the detector side, we have: e1x e U p ( a )U b ( m ,2BLE 2 )U p ( p ) 0 x e e 1y 0y (2.3) where the subscripts a, m and p stand for analyzer, Kerr material and polarizer, respectively. As shown in Figure 2.2, the y-axis is usually so chosen that it coincides with the direction of applied HV field, i.e. ψm=0 in Equation (2.3). Then, e1x sin 2 a e sin cos a a 1y 0 sin 2 p sin a cos a 1 i 2BLE 2 cos 2 a 0 e sin p cos p i 2BLE 2 sin 2 a sin 2 p sin sin 2 e a p 4 2 i 2BLE 2 sin sin 2 e cos 2 a sin 2 p p a 2 2 A12 e0 x A 11 A21 A22 e0 y 2 sin p cos p e0 x cos 2 p e0 y e i 2BLE cos 2 p sin 2 a e0 x 2 2 e0 y sin 2 a sin 2 p i 2BLE 2 2 2 e cos a cos p 4 sin 2 a sin 2 p Further, if the polarization angle of the laser output is 2 (2.4) (with respect to y-axis, i.e. ), the light intensity ratio is therefore: * e1x A* A21 A11 A12 e0 x (e1x , e1y ) (e0x , e0 y ) 11 * * e1 y A12 A22 A21 A22 e0 y I1 e I0 e0 x 0x (e0 x , e0 y ) (e0x , e0 y ) e0 y e0 y A 2 A21 2 A11 A12 A21 A22 sin e e0 (sin , cos ) 11 2 2 A A A A cos 0 A A 22 21 12 22 12 11 sin e0 e0 (sin , cos ) cos A11 2 A21 2 A11 A12 A21 A22 sin (sin , cos ) 2 2 A A A A A12 A22 cos 22 21 12 11 20 (2.5) In general, Equations (2.4) and (2.5) expanded in terms of the angles and basic parameters will be very complicated. In this chapter, we focus on a special case with crossed polarizers, i.e. and . Then according to Equation (2.4), , and Equation (2.5) is simplified: 1 cos(2BLE 2 ) 1 cos(2BLE 2 ) sin I1 4 4 (sin , cos ) 2 2 I0 1 cos(2BLE ) 1 cos(2BLE ) cos 4 4 2 2 1 cos(2BLE ) (sin cos ) (sin cos ) 2 sin 2 (BLE 2 ) 4 2 (2.6) In Equation (2.6), the ratio of output and input light intensities for a linear polariscope with crossed polarizers, which is measurable in experiments, depends on the initial polarization angle of the incident laser, . It is straightforward to show that by setting one can maximize the light intensity at the detector side, which is: I1 sin 2 (BLE 2 ) I0 (2.7) In this section, we only consider the simplest case. For the comparison of various polariscopes and parameter settings, see Section 3.2. 21 2.3 Experimental setup The experimental setup illustrated in Figure 2.3 consists of optical, electrical and control subsystems. A test cell with transformer oil and a pair of parallel-plate electrodes (gap spacing mm, length m) inside is the intersection of the optical and electrical subsystems. Vacuum and filter systems remove the bubbles and particles in the oil that may cause premature electrical breakdown and reduce optical detection accuracy. Figure 2.3. Experimental setup for Kerr electro-optic field mapping measurements. The diameter of the pulsed laser beam (wavelength 532 nm) is 7.6 mm and 98% linearly polarized. The polarizers (P0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. P0 is used to attenuate the laser to avoid saturating the CCD camera. The transmission angles of P and A are 45°and −45°with respect to the x-axis (crossed polarizers). The CCD camera is a megapixel back-illuminated EMCCD with single photon detection capability. The imaging area (8×8 mm2) covers the 2 mm gap (~250 pixels across). 22 The Quantel Ultra Laser is a rugged Q-switched ND:YAG oscillator that is ~98% linearly polarized with pulse energy of 30 mJ @ 532 nm, 20 Hz maximum repetition rate, and less than a 6 mrad beam divergence. The output beam is at 1064 nm wavelength that then goes through a manual variable attenuator. The attenuated beam goes to the frequency doubler that provides the 2nd harmonic that is used for the test measurements. The diameter of the pulsed laser beam (wavelength 532 nm) is 7.6 mm. Any reflections from optical or other components back into the laser head should be prevented as it can severely damage the components. The reflected light back into the laser can increase the laser energy internal to the head causing stresses, high heating, and in some case melting of optical components. A linear polariscope (no quarter wave plates) with crossed polarizers P and A is used to measure the Kerr effect. The polarizers (P0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. P0 represents a series of polarizers used to attenuate the laser to avoid saturating the CCD camera. To realize the optimum measurement condition required by Equation (2.7), the last attunuation polarizer (closest to P) has its transmission axis fixed at 45°with respect to the x-axis, while other P0 polarizers can be rotated to control the transmitted light intensity). The transmission angles of P and A are 45°and −45°with respect to the x-axis (crossed polarizers). The light intensity is measured by an Andor Technology iXonEM+ electron multiplication charge coupled device (EMCCD) camera Model DU-885K. A megapixel backilluminated EMCCD, the camera is cooled to -80°C, and sensitive enough to output 1 electron per photon detected called a “count”. The camera can be triggered internally via the computer or externally via a 5V trigger pulse. The exposure time can be set internally and triggered externally if needed. The camera saturates above 16,000 photons (at a gain of 3.5) or 23 approximately 55,000 counts, and careful attention to not overexpose the camera must be taken. If overexposure occurs the signal pixels will be capped at the saturation level. This means that if any additional light is passed to the sensor, then no changes in pixel values will occur when there should be pixel value changes. The imaging area of the CCD camera (8×8 mm2 having an active pixel size array of 1004×1002 yielding an approximate pixel size of 8µm) covers the 2 mm gap (~250 pixels across). The CCD imaging area is ~1 m away from the test cell in order not to receive the scattered light (not propagating along z direction) which makes the gap look wider and generates extra patterns in the recorded light field (we will discuss this later in Chapter 3 and Chapter 5). The instruments of HV generation and measurement system include power supplies, capacitors, capacitive dividers, oscilloscope, function generators, and related items. The Hipotronics Marx Generator 300 kV provides the HV pulses and is configured with utility grade capacitors to modify the rise and decay times of the pulses. The capacitive voltage divider is a Pearson Model VD-500A. The frequency range is 15Hz to 2MHz, usable rise time of 200 nanoseconds, and 5068:1 voltage division ratio in oil. The sensors are measured by LabVIEW hardware and the HP Infinium Oscilloscope 500 MHz 1 GSa/s. The digital delay generator Model 113DR (MOD) is used to provide delay and trigger timing for various pieces of the test setup. The function generators are either Agilent Model 33220A 20MHz Single Channel, HP Model 33120A 15MHz Single Channel, or Agilent Model 33522B 30 MHz Two Channels with arbitrary waveform generation and delay triggering capability. In this chapter, the HV pulse from the Marx generator has a rise time of ~250 µs, and total duration of ~20 ms. A LabVIEW controller is designed to monitor the HV waveforms from the capacitive divider and generate pulses to trigger the pulsed laser and the CCD camera 24 at certain instantaneous voltages. Representative waveform of the HV pulse is presented in Figure 2.4. Two trigger signals generated by LabVIEW are: (1) for CCD exposure start and pulse laser flashlamp trigger, the controller outputs a trigger pulse when the instantaneous voltage (Uins) passes a preset value (in Figure 2.4, it is 20 kV); (2) for pulse laser Q-switch trigger, the controller sends a signal after a time delay, which should be in the range of 100 to 140 µs to guarantee the output power stability of the laser. Figure 2.4. Representative waveform of the HV pulse from the Marx generator measured by the 5068:1 capacitive divider. Two triggering pulses are generated by the LabVIEW controller to first trigger the camera and the flashlamp and then after 0.1 ms delay trigger the Q-switch to output the laser pulse. Figure 2.5 below shows the view when looking into the window of the test cell. The actual direction of the x-axis is horizontal, and the electrodes are aligned vertically in the transformer oil filled test cell. 25 To measure the fringing field, the laser beam and the CCD imaging area shown in Figure 2.5 should move correspondingly. Although the exposure time of the CCD is set to be several hundred microseconds, the effective exposure time of the CCD is the laser pulse duration (several nanoseconds). Window of the Test Cell Light Propagation Laser Beam Diameter 7.6 mm HV Electrode 0 d=2 mm ~250 pixels Grounded Electrode Imaging Area 8 8 mm 2 Effective Exposure Time: < 0.1 µs x Figure 2.5. The view when looking into the window of the test cell. To measure the fringing field, the laser beam and the camera should move correspondingly. The effective exposure time of the CCD is the laser pulse duration (several nanoseconds). 26 2.4 Results and discussions In Section 2.2, using Jones’ calculus, , the ratio of transmitted light intensities of A and P0 (see Figure 2.3) as a function of , has been given in Equation (2.7), which is the theoretical result in an ideal experimental setting. In fact, if taking into consideration the light power loss due to reflection from optical surfaces and absorption in materials, Equation (2.7) should be re-written in a more general form: (2.8) where is the fraction of light power loss (independent of HV and light polarization). According to Equation (2.8), should be zero corresponding to crossed polarizer output without HV Kerr effect. However, the laser is not 100% linearly-polarized, and when no HV is applied, a very small portion of light intensity, denoted by , can propagate through the crossed polarizers into the imaging area of the camera. As will be shown later, the increase in light intensity due to the Kerr effect in transformer oil is of the same order or even less than . Therefore, appropriate treatment and quantitative characterization of will be an important part of the measurements. Preliminary measurements are conducted to determine the intensity and polarization state of the leaked light. The main observations are stated below: (A) When there is no applied HV, it is found that is proportional to ( can be tuned by adjusting the transmission angle of P0 polarizers), i.e. where , is the fraction of leaked light intensity. (B) When inserting a polarizer P3 between A and the CCD and then adjusting its transmission angle, there is no significant variation in 27 (however, slight differences may be detected due to the laser beam fluctuation). Further, inserting a quarter wave plate between A and P3 and then adjusting the angle of its optical axis, again no variation in is detected, indicating that the leaked light is basically unpolarized and no Kerr effect should be expected from this part of light intensity. According to these observations, the actual signals of the Kerr effect (the numerator and denominator on the left side of Eq. (2.8)) should be and and , instead of . Equation (2.8) is transformed as: (2.9) where has been assumed (for E~10 kV/mm, ). The degree of polarization of the laser provided in the manufacturer test report is 98.3%, which means or . Some measurement results with a space-charge free field in the mid-region of the gap will first be presented. The characteristic time for the appearance of strong space charge effects is the migration time τm of charge carriers across the gap (spacing d) based on mobility µ: τm=l/(µE). Given E~107 V/m, d=2 mm, and µ~10-7 m2/Vs (called electrohydrodynamic mobility; ion mobility is 1-2 orders lower) [2-10], then τm~2 ms. If measurements are taken at t = 0.1 ms (t = 0 defined as the beginning of the HV pulse), the field over the majority of the gap should be uniform due to a negligible space charge distribution. The intensity distributions of , and as , as instantaneous voltage are shown in Figures 2.6(a), (b), and (c), respectively. We see that the light intensity distribution of the laser beam has a Gaussian profile instead of a uniform one. Using the CCD area detector, we record and process the light intensity and its variation at each pixel within the region of interest. Besides, from shot to shot, 28 the light intensity distribution has fluctuations that cannot be neglected. In view of this, under each experimental condition, the measurement is repeated 100 times and the data is averaged to reduce random fluctuation. (a) (b) (c) Figure. 2.6. Measurements of uniform field without space charge between two aluminum electrodes in transformer Maximum deviation from oil. The position of the imaging area is shown in Figure 2.5. (a) The distribution of I1(0), where the dark regions to uniform field left and right of the illuminated area are electrodes. The light intensity (counts of electrons at a pixel) is represented Difference between applied by the colormap. (b) The distribution of I1(E) − I1(0) when the instantaneous voltage (Uins ) is 16 kV; and the voltage and integration of camera is triggered at 0.1 ms. (c) The distribution of I1(E) − I1(0) at Uins=24 kV. In Figure 2.7, the ratios of and (as on the left side of Equation (2.9)) (e) (d) under various measured field (f) values (0, 4, 6, 8, 10, 12, 14 kV/mm) are calculated and then fitted with a 4th power function: . The MATLAB curve fitting tool gives the coefficient with 95% confidence bounds: (1.255±0.016)×10−4, and the goodness of fit is indicated by the R-square (0.9997). Since according to Equation (2.9), one can evaluate the Kerr constant of transformer oil at 532 nm: . In a previous work [2-8], we determined the Kerr constant of the used transformer oil at 632.8 nm as optic effect predicts that . Classical theory of the Kerr electro- (Havelock’s law) [2-11]. Our measurement results presented above are in good agreement with the theory. 29 Figure 2.7. Ratio of I1(E) − I1(0) and I1(0) from the averaged data and power function (exponent=4) fitting. Figure 2.8. Measured field distributions across the gap corresponding to Uins=24 and 16 kV. 30 In Figure 2.8, based on Equation (2.9) with the measured Kerr constant, electric field distributions across the gap under Uins=24 and 16 kV are presented. The dashed lines in Figure 2.8 are the theoretical uniform field distribution. The measured field distribution is not perfectly uniform; the deviation from uniformity is possibly due to the laser beam fluctuation and other random processes in the system. There are two measures to characterize the error of the measurement results: (i) the maximum deviation of the measured field from theoretically-predicted uniform field (dashed lines), which reflects the magnitude of the effect of randomness and is an indicator of measurement sensitivity; and (ii) the difference between the instantaneous voltage and the integration of the measured electric field over the gap, which, as a basic check of the applicability and accuracy of experimental principles and methods, defines the measurement reliability. Figure. 2.9. Relative errors of the measurement results: the maximum deviation of the measured field from uniform field, and the difference between the instantaneous voltage and the integration of the measured field over the gap. 31 The relative errors of the two types under various voltages are plotted in Figure 2.9. The relative error of type (ii) is lower than that of type (i) because the former is essentially an average of the latter over the gap which reduces the random fluctuations. When Uins is less than 10 kV, the maximum deviation from uniform field is ~30%, meaning that the light intensity increase due to the Kerr effect is heavily contaminated by the random fluctuation of the laser beam. As Uins increases, both errors become lower. While the relative error of type (ii) can be as low as 2.5%, the random fluctuations still bring in >5% relative error of type (i), even if the applied voltage is very close to the breakdown threshold. Type (i) error is the primary factor that impedes the improvement of measurement sensitivity. This can be better demonstrated by taking images of the region near the edge of the electrodes, where the non-uniform field is called the fringing field. In Figure 2.10, the Oy axis is defined as the midline of the gap, i.e. the two sides of the axis are symmetric. Although the rounded edges of the two electrodes are not geometrically identical, the fields at the points on the Oy axis are approximately along the x-direction, and the principle of Kerr measurements for uniform gap (e.g. Equation (2.9)) also applies to field mapping along the Oy axis. Comparing Figure 2.10(b) with Figure 2.10(a), it is found that the increase in light intensity is higher inside the gap than outside of the gap. From Figure 2.11, one can see that, the measured electric field along the Oy axis generally agrees with the numerical solution in Maxwell® 2D. The maximum deviation between measurement and the numerical results in the range of 0< y <1.5 mm as a function of Uins is plotted in Fig. 2.12. The error bars come from the standard deviation of 100 repeated measurements. 32 O y (b) (a) Figure 2.10. Measurements of space-charge free fringing field with two stainless steel electrodes in transformer oil. The laser beam is shifted to illuminate the fringing area and the position of the CCD imaging area is adjusted correspondingly. (a) The distribution of I1(0). The profiles of the rounded edges of the electrodes can be seen. The light intensity (counts of electrons at a pixel) is represented by the colormap. (b) The distribution of I1(E) − I1(0) when the instantaneous voltage (Uins) is 24 kV and the camera is triggered at 0.14 ms. 24 kV 16 kV y (mm) (c) Figure 2.11. Measured field distributions along Oy axis indicated in Figure 2.10 corresponding to Uins=24 and 16 kV. The dot-dashed lines are numerical simulation results. 33 Figure 2.12. Dependence of the relative error of the measurement results in the range of 0< y <1.5 mm on Uins. Under lower voltages, the errors due to randomness are more significant, while the requirement on measurement sensitivity is higher. Therefore a tradeoff exists between sensitivity and error. For example, if one wants to take measurements under Uins=16 kV, the highest sensitivity, limited by the randomness-induced error, will be ~10%, which means that the measurements do not have enough ‘contrast’ to consistently distinguish fields unless their difference in intensity is over ~0.8 kV/mm. In order to further improve the Kerr measurement sensitivity, it is necessary to identify and correct (if possible) various sources of randomness in the system. It has been demonstrated that the Kerr technique can successfully map the space-charge free field with satisfactory accuracy when the mean field across the gap kV/mm. Whether or not the same method can be extended to electric field with space charge is to be examined below. Since the mechanisms of space charge generation and transport are unclear, 34 the measured data cannot be verified by numerical models. Nevertheless, we will illustrate that the mapped field from the Kerr measurements is physically reasonable and consistent. With the electric field distribution measured, the space charge density from Gauss’ law ( , can be solved is the dielectric constant of transformer oil). As shown in Figure 2.13, aluminum electrodes inject negative charges (average charge density is 0.037 C/m3) into the gap, while the charge injection from titanium electrodes is much weaker. t = 0.7 ms, Uins = ±28 kV – + Figure 2.13. Measurements with same-material electrode pairs under HV pulses of both polarities. The position of the imaging area is the same as Figure 2.5. The camera is triggered at 0.7 ms with the instantaneous voltage Uins= ±28 kV. For both polarities, the anode is located at x/d=0, while the cathode is located at x/d=1. The results presented in Figure 2.13 indicate that since the two electrodes are made from the same material (or approximately speaking, two identical electrodes), switching the polarity (keeping other parameters of the applied voltage unchanged) should not affect the charge 35 injection and transport behavior. This physical consistency implies that the presence of space charge in our experimental configurations has little effect on the physical processes involved in the Kerr electro-optic effect and does not undermine the validity of the basic principles of the field mapping measurement. In this chapter, we demonstrate both quantitatively and qualitatively that Kerr electrooptic measurements with a high-sensitivity CCD camera can be used for electric field mapping. Measurement accuracy and reliability for uniform and fringing space-charge free fields and field with space charge have been evaluated. Generally speaking, the relative errors will be reduced as the voltage increases. This may not be true when the voltage approaches the breakdown threshold, since more uncertainties would be introduced due to high-field conduction and pre-breakdown phenomena in the liquid dielectrics. To further improve the sensitivity of the measurements, we need to identify and quantify various sources of noise in the experimental system, including optical, electro-optical, and electrochemical processes. Image processing techniques may also be helpful to enhance the data quality. The most straightforward application of image processing algorithms in our measurements is edge detection, i.e. identification of the electrode surfaces in the images taken by the CCD camera. This would be more demanding when the oil gap is smaller, since the same edge detection inaccuracy (e.g. 5 pixels) takes up a larger portion of the gap. 36 References [2-1] A. Denat, “Conduction and Breakdown Initiation in Dielectric Liquids”, in Proc. ICDL, Trondheim, Norway, Jun. 26-30, pp. 1-11 (2011). [2-2] T. J. Lewis, “Basic Electrical Processes in Dielectric Liquids”, IEEE Trans. Dielectr. Electr. Insul. 1, 630 (1994). [2-3] I. Adamczewski, Ionization, Conductivity and Breakdown in Dielectric Liquids (Taylor&Francis, London, 1969). [2-4] U. Gäfvert, A. Jaksts, C. Törnkvist, and L. Walfridsson, “Electrical Field Distribution in Transformer Oil”, IEEE Trans. Electr. Insul. 27, 647 (1992). [2-5] M. Zahn, L. L. Antis, and J. Mescua, “Computation Methods for One-Dimensional Bipolar Charge Injection”, IEEE Trans. Ind. Appl. 24, 411 (1988). [2-6] V. Y. Ushakov (ed.), Impulse Breakdown of Liquids (Springer-Verlag, Berlin, 2007). [2-7] M. Zahn, “Optical, Electrical and Electromechanical Measurement Methodologies of Field, Charge and Polarization in Dielectrics”, IEEE Trans. Dielectr. Electr. Insul. 5, 627 (1998). [2-8] X. Zhang, J. K. Nowocin, and M. Zahn, “Effects of AC Modulation Frequency and Amplitude on Kerr Electro-Optic Field Mapping Measurements in Transformer Oil”, in Annual Report of CEIDP, Montreal, Canada, pp. 700-704 (2012). [2-9] E. Collett, Field Guide to Polarization (SPIE Press, Bellingham, 2005). [2-10] M. Zahn, “Conduction and Breakdown in Dielectric Liquids”, in Wiley Encyclopedia of Electrical and Electronic Engineering Vol. 20, pp. 89-123 (1999). [2-11] J. W. Beams, “Electric and Magnetic Double Refraction”, Rev. Mod. Phys. 4, 133 (1932). 37 38 3 Kerr electro-optic field mapping study of the effect of charge injection on the impulse breakdown strength of transformer oil Synopsis The smart use of charge injection to improve breakdown strength in transformer oil is demonstrated in this chapter. Hypothetically, bipolar homo-charge injection with reduced electric field at both electrodes may allow higher voltage operation without insulation failure, since electrical breakdown usually initiates at the electrode-dielectric interfaces. To find experimental evidence, the applicability and limitation of the hypothesis is first analyzed. Impulse breakdown tests and Kerr electro-optic field mapping measurements are then conducted with different combinations of parallel-plate aluminum and brass electrodes stressed by millisecond duration impulse. It is found that the breakdown voltage of brass anode and aluminum cathode is ~50% higher than that of aluminum anode and brass cathode. This can be explained by charge injection patterns from Kerr measurements under a lower voltage, where aluminum and brass electrodes inject negative and positive charges, respectively. This work provides a feasible approach to investigating the effect of electrode material on breakdown strength. 39 3.1 Introduction Dielectric liquids used in power system apparatus and pulsed power technology have their performance affected by injected space charge that distorts the electric field distribution between electrodes. For highly purified water, Kerr electro-optic measurements and electrical breakdown tests have shown that the magnitude and polarity of injected charge and the electrical breakdown strength depend strongly on electrode material combinations and applied voltage polarity [3-1]. Figure 3.1 (from [3-2]). Space charge distortion of the electric field distribution between parallel plate electrodes with spacing d at voltage V so that the average electric field is E0=V/d. Four simplest possible configurations are shown: (a) no space charge; (b) unipolar positive or negative charge; (c) bipolar homocharge; (d) bipolar heterocharge. Figure 3.1 shows four simplest configurations of space charge distorted electric field distribution between parallel plate electrodes with spacing d at voltage V. The electric field is 40 uniform at the average field E0 when there is no space charge (Figure 3.1(a)). In Figure 3.1(b), according to Gauss’ law, unipolar positive/negative charge distribution has the electric field maximum at the cathode/anode, thus possibly leading to electrical breakdown at lower voltages. For bipolar homocharge distribution shown in Figure 3.1(c), the positive charge region is near the anode and negative charge near the cathode, so that the electric field is lowered at both electrodes and is largest in the central region. In contrast, bipolar heterocharge distribution (Figure 3.1(d)) has the electric field enhanced at electrodes and depressed in the central region. It has been hypothesized that bipolar homo-charge injection (positive charge injected at the anode and negative charge injected at the cathode) with reduced electric field at both electrodes may allow higher voltage operation without insulation failure, since electrical breakdown usually initiates at the electrode-dielectric interfaces [3-1,3-2]. At first glance, the statement seems true and self-evident. Nevertheless, this problem is actually very complicated and remains poorly understood for systems of practical interest. Firstly, the electric field profile across the gap, the integration of which equals to the instantaneous voltage, can actually be very complex. According to Gauss’ law, the charge density is proportional to the divergence of electric field, which is the slope of the onedimensional electric field profile between parallel-plate electrodes [3-2]. The positive (negative) slope at the anode (cathode) does not ensure that the local electric field is lower than the space charge free field. The curves in Figure 3.1 are only the simplest possible cases. The electric field distribution in the central region of the gap may exhibit more up-and-down patterns. Secondly, reduced electric field at both electrodes may not correspond to improved breakdown strength. For example, suppose electrode material #1 has homo-charge injection and material #2 has no charge injection, but meanwhile the intrinsic (i.e. space charge free) 41 breakdown strength of #1 is much lower than that of #2. In this case, the hypothesis may not hold since homocharge corresponds to lower breakdown voltage, suggesting that the intrinsic breakdown strength should be considered as an important precondition. Besides, strong charge injection currents, usually a destabilizing and uncontrollable factor in insulation configurations, can cause instability at electrode surfaces [3-3]. It is also worthwhile to point out that, the hypothesis is based on the dc steady state. However, under a strong dc electric field, turbulent flow can be induced due to electrohydrodynamic instability [3-4]. That is, a stable dc steady state may not even exist. On the other hand, when the applied high voltage is a short pulse (no induced flow), the validity of the hypothesis is questionable since charge injection may be irrelevant to breakdown. The ASTM D3300-12 standard test method for dielectric breakdown voltage in insulating oils under 1.2/50 μs lightning impulse condition is performed using a tip opposing a grounded sphere. The breakdown is preceded by the propagation of streamers emerging from the highvoltage tip electrode, while the space charge behavior is negligible before the streamer inception [3-5]. Finally, for transformer oil, the most common industrial insulating liquid, experimental evidence is on demand. Published works on the effect of electrode materials on breakdown strength are largely empirical, and theoretical analysis based on electronic, mechanical and thermodynamic characteristics of the metal is not in satisfactory agreement with the experimental results [3-6]. It is partly because factors that affect the breakdown strength significantly, such as gap geometry, applied waveform, test procedure, the state of electrode surfaces and the quality of the transformer oil, vary in different works. Measurement method is also a limiting factor: only monitoring voltage/current waveforms at electrical terminals cannot 42 provide detailed information on electric field distribution and space charge dynamics in transformer oil during the conduction and pre-breakdown phases. In this chapter, experiments are designed to examine the applicability of the hypothesis. The measurement of the electric field distribution is made possible by the Kerr electro-optic field mapping technique. Using a high sensitivity CCD (charge-coupled device), our recent work [3-7] demonstrated the reliability of Kerr measurements with high voltage pulsed transformer oil, which had been a bottleneck due to the low Kerr constant of transformer oil and the low sensitivity of old detectors. As a continuing work, different combinations of electrode materials will be tested in this chapter to find the connections between impulse breakdown strength and charge injection pattern. The duration of the applied high voltage impulses should be long enough for the space charge effect to manifest, and meanwhile, be as short as possible to minimize induced flow in the dielectric liquids which disturbs the optical detection. 43 3.2 Optimization of Kerr experimental configurations In Section 2.2, the basic principle of Kerr measurement has been introduced based on a linear polariscope with crossed polarizers. Actually, there are four different polariscope configurations: linear, pre-semi, post-semi and circular (Figure 3.2). In each of them, transmission axes of the polarizer and the analyzer can either be crossed or aligned. (a) Linear polariscope (b) Pre-semi polariscope (c) Post-semi polariscope (d) Circular polariscope Figure 3.2. Four polariscope configurations: (a) linear; (b) pre-semi; (c) post-semi; (d) circular. 44 In this section, we are going to discuss which one is the optimum configuration for practical measurements in the sense that it yields the highest accuracy and stability. There are also many other factors that will reduce the accuracy and stability of the measurement results: optical components not perfect or not precisely adjusted; impurities and flow of the dielectric liquid; fluctuations of laser intensity; thermal noise within the CCD camera; environment. Although at the current stage we only focus on the optimization of the measurement configuration, we should not neglect the influence of these factors. We start from a linear polariscope where the output/input light intensity ratio can be calculated according to Equations (2.3)−(2.5). With the help of mathematical software, we can avoid complicated symbolic computation and easily obtain useful numerical results. 1. Aligned polarizers ( ) 1.5 0.9 1 0.8 0.7 (radians) 0.5 0.6 0.5 0 0.4 -0.5 0.3 0.2 -1 0.1 -1.5 -1.5 -1 -0.5 0 0.5 1 1.5 (radians) p Figure 3.3. Numerical results of the intensity ratio when 45 , and vary from to . The Kerr constant of transformer oil is . If the average electric field and the electrode length is shift , then it is estimated that the Kerr phase . However, when the voltage is applied, due to space charge, the field may not be uniform across the gap. If we want to get the non-uniform field distribution, we must at least be able to distinguish least be able to detect the change of If , and , and as small as vary from to is shown in Figure 3.3. In cases with , that is, the measurement should at . , the contour plot of the intensity ratio the intensity ratio is very close to 1. When , since the polarizer would let little light go through, the intensity ratio is essentially zero. The two cases yield trivial results, and thus should be avoided. Somewhere in between seems more appropriate. The appropriateness is based on two considerations: the contrast, i.e. the capability to distinguish the light intensities for different values of ; and the error behavior, i.e. the changes in the results as some parameter of the system has small deviations from the theoretically specified value. Table 3.1. Numerical results of as 0.8535 0.7499 0.5000 0.2500 0.1464 , and 0.8534 0.7498 0.4998 0.2499 0.1464 0.8532 0.7495 0.4996 0.2498 0.1464 in the range of 0.8529 0.7491 0.4992 0.2497 0.1463 In Table 3.1, we present the numerical results of the intensity ratio , and in the range of . 0.8525 0.7486 0.4988 0.2495 0.1463 as , from which one can see that when , the contrast is better than (by comparing the difference between 46 and in each case). Numerical results of the intensity ratio as are given in Table 3.2. Now we assume the two polarizers are not perfectly aligned, which means that there may be a small difference ( changes in ( ) between and . The are also calculated and expressed in percentage of the values in ideal settings ). From Table 3.2 we can see that when measurement seems more stable than , the variation is smaller and the . Table 3.2. Numerical results as , and 0.8535 0.7499 0.5000 0.8532 0.7495 0.4996 0.8525 0.7486 0.4988 . Variation (%) 2.437 2.440 2.440 2.461 2.454 2.441 2.475 2.471 2.445 0.8327 0.7316 0.4878 0.8322 0.7311 0.4874 0.8314 0.7301 0.4866 Thus in principle, it seems that has a deviation of leads to the result with maximum contrast and best error behavior. However, to detect very small modulation effects , the contrast of aligned polarizers is far from adequate. The saturation level of each pixel in the CCD camera is 50000 counts (of electrons). The fluctuation level of each pixel is at least 10 to 20 counts, which means that, in this configuration, we cannot distinguish and ( ( ), ( ). For example, from the results shown in Table 3.1, the difference 47 ) between and is only , which corresponds to only 20 counts, approximately on the background noise level (mainly due to the fluctuations of the laser and internal errors of the CCD). Hence we cannot obtain reliable non-uniform field distribution across the gap in this configuration. 2. Crossed polarizers ( If , ) and vary from to , the contour of the intensity ratio is shown in Figure 3.4. x 10 -5 1.5 9 1 8 7 (radians) 0.5 6 5 0 4 -0.5 3 2 -1 1 -1.5 -1.5 -1 -0.5 0 0.5 1 1.5 0 (radians) p Figure 3.4. Numerical results of the intensity ratio when In Figure 3.4, it is obvious that , and vary from to . yields the maximum output light intensity. This is useful because with crossed polarizers the transmitted light intensity is always very low 48 for low Kerr constant materials like transformer oil. The output light intensity needs to be high enough to be detectable. 2.5 x 10 -3 2 I 1/I 0 1.5 1 0.5 0 0.02 0.03 0.04 0.05 0.06 0.07 0.08 0.09 0.1 (radians) Figure 3.5. Numerical results as , and varies from to rad. 0.03 =0.02 =0.06 =0.1 0.025 I 1/I 0 0.02 0.015 0.01 0.005 0 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 - -/2 (radians) p a Figure 3.6. Numerical results as , and 49 varies from to . In the case with , we calculate the intensity ratio electric field or the phase retardation between the values of as a function of the . The results are plotted in Figure 3.5. The difference when and is about 1/1000, which corresponds to about 100 counts (CCD pixel information), higher than that of aligned polarizers (20 counts). However, with crossed polarizers, can be set higher than the saturation level of the CCD (50000 counts), since the detected light intensity incident light intensity (with aligned polarizers, is only a very small fraction of the ). Typically we can choose to be 3 to 5 times of the saturation level, which results in a further 3 to 5 times enhancement in the measurement sensitivity. It can be concluded that, the contrast of crossed polarizers is much better than that of aligned polarizers. This also explains why we used this configuration in Chapter 2. In practice, it may be very difficult to make sure that the polarizers are perfectly crossed. As shown in Figure 3.6, if the two polarizers are not perfectly crossed, the deviation in light intensity ratio can be much greater than the value in ideal settings. For example, when and to (about ), the error will be over 10% of the result corresponding . The magnitude of the error also seems to increase nonlinearly as the imperfection in alignment is augmented. While compared to aligned polarizers, crossed polarizers have higher contrast and sensitivity, their poor error behavior of the crossed polarizers may be a limiting factor of the reliability of the results when we take Kerr measurements. Next, we will try crossed polarizers with a quarter wave plate inserted (pre-semi polariscope). 50 3. Effect of quarter wave plates (pre-semi polariscope) Since we have known that the contrast and error behavior of the linear polariscope are not adequate for the measurement of small signals, the next thing we tried is to insert a quarter wave plate between the polarizer and the test cell (called pre-semi polariscope) and see if there is any improvement. In the discussion below, we fix the polarization angle of the laser output to . For quarter wave plates, the slow axis is at angle ψ with respect to the y-coordinate and the slow wave is retarded by exout cos out e sin y in phase: sin 1 0 i/2 cos 0 e cos sin exin sin exin U q ( ) in e cos einy y (3.1) In the experimental setting shown in Figure 2.2, when a quarter wave plate is inserted between the polarizer and the test cell, we have: e1x e U p ( a )U b (0, )U q ( )U p ( p ) 0 x e e 1y 0y (3.2) The matrix elements in Equations (2.4) and (2.5) should now be modified correspondingly. , ψ and For crossed polarizers, if vary from to , the contour of the intensity ratio is shown in Figure 3.7. In Figure 3.7, the optimum case with highest output light intensity is when ψ function of the phase retardation and . In this case, we calculate the intensity ratio as a . The results are plotted in Figure 3.8. 51 1.5 0.45 1 0.4 0.35 (radians) 0.5 0.3 0 0.25 0.2 -0.5 0.15 0.1 -1 0.05 -1.5 -1.5 -1 -0.5 0 0.5 1 1.5 (radians) p Figure 3.7 Numerical results of the intensity ratio when , , ψ and vary from to . Comparing Figure 3.7 with Figure 3.4 (without quarter wave plate), we can find a significant improvement on the output light intensity (from 10-3 to 10-1 ). However, this does not mean that the Kerr measurement sensitivity is also enhanced by two orders, because the sensitivity requires a clear cut between the signals with and without Kerr electro-optic effect. From Figure 3.8, it can be seen that the intensity ratio grows almost linearly with the phase retardation (or similarly . There are detectable differences in and ). If between and (counts of electrons), this difference (around 0.01) can be 500 counts of electrons, much greater than the noise level (20 counts). Hence the sensitivity of the pre-semi configuration is satisfactory. Next we will check its error behavior. 52 0.555 0.55 0.545 0.54 I 1/I 0 0.535 0.53 0.525 0.52 0.515 0.51 0.505 0.02 0.03 0.04 0.05 0.06 0.07 0.08 0.09 0.1 (radians) ,ψ Figure 3.8 Numerical results of the intensity ratio when , , from to rad. 0.555 0.55 0.545 0.54 I 1/I 0 0.535 0.53 0.525 0.52 0.515 =0.02 =0.06 =0.1 0.51 0.505 -0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2 - -/2 (radians) p a Figure 3.9 Numerical results of the intensity ratio as and 53 varies from to . In Figure 3.9, we present the numerical results of the intensity ratio and varies from to as . As shown in Figure 3.9, if the two polarizers are not perfectly crossed, the magnitude of the error is negligible compared with that of the signal. For instance, when and lower than 1% of the result of (about ), the error is . Furthermore, if the Jones’ matrix for a polarizer (see Equation (2.1)) becomes: Exout cos out E sin y where 0 cos sin x cos 0 1 y sin sin Exin cos E yin (3.3) are small quantities to characterize imperfections in the polarizer material. We recalculate the above case. We find that, if smaller than 1%, the imperfection of the polarizers contributes little to the measured data. The main conclusion for the post-semi polariscope (Figure 3.2(c)) is similar to the presemi polariscope, and the analysis of the circular polariscope (which can be used to eliminate isoclinic lines if there are any in the measurement) yields similar results to that of the linear polariscope. For this reason, we do not discuss here these two types of polariscope in details. The work done in this section indicates that pre-semi polariscope with crossed polarizers will be an optimized experimental configuration for Kerr electro-optic field mapping measurements with low Kerr constant dielectric liquids like transformer oil. Its sensitivity (contrast) and consistency (stability) under imperfection have been shown to be better than those of linear polariscope. 54 3.3 Experimental procedure We use a 0.25/20 ms high voltage pulse (the detailed reason will be discussed later). The fitted curve for the waveform can be expressed in double-exponential form: , where is approximately the peak voltage, ms and μs are two constants. The transformer oil is lab-aged Shell DIALA A oil without dehydration or high-standard degassing/filtering. Although there are a vacuum pump and an oil filter in the experimental setup, their function is to remove visible bubbles and particles in the oil that may cause premature electrical breakdown and reduce optical detection accuracy. The electrodes have been rinsed with reagent alcohol and conditioned in the oil by slowly increasing dc voltages (no breakdown) for hours. The impulse breakdown voltages of the transformer oil filled gap (width 2 mm) between parallel-plate electrodes (4 different combinations of brass 360 and aluminum 2024, both with approximately the same surface roughness µm) are tested using the rising- voltage method [3-8]. During the breakdown test, we apply the impulse waveform starting from ~25 kV. At each voltage level, apply 3 impulse waves and allow at least 30 s between each test. is increased in steps of 1~2 kV until breakdown occurs. After each breakdown, we clean the electrode surfaces and run the filter and then the vacuum to reset the test cell. The experimental setup for Kerr measurements is illustrated in Figure 3.10. The diameter of the laser beam (wavelength 632.8 nm, linearly polarized) is 0.5 mm. The 20× beam expander expands the laser beam to about 10 mm in diameter. The polarizers (P0, P, A) have an extinction ratio 500:1 and diameter of 10 cm. Plano-convex lenses L1 and L2 are 25.4 mm in 55 diameter and the effective focal length is 50.2 mm . The Andor iXon camera is a megapixel back-illuminated EMCCD with single photon detection capability. The imaging area (8×8 mm2) covers the 2 mm gap (~250 pixels across). The CCD camera measures the light intensity of the laser beam coming through the presemi polariscope with crossed polarizers (P and A). Polarizer P0 is used to ensure the linear polarization state of the expanded laser beam and to attenuate the laser to avoid saturating the CCD camera. A quarter-wave plate (Q) is inserted between P and the test cell (pre-semi polariscope) to increase measurement sensitivity. The angle of polarization of the laser output is 45° (with respect to the x-axis); the transmission angles of P and A are 45° and −45°, respectively; for the quarter-wave plate (Q) and the transformer oil-filled gap, the slow wave is polarized along the x-axis, with phase retardation and is the Kerr constant of transformer oil [3-9], along the light path, and where m is the electrode length is the electric field. Figure 3.10. Experimental setup for Kerr electro-optic field mapping measurements. The ratio of light intensities detected by the CCD camera with and without high voltage 56 is given by [3-2,3-9], from which the electric field intensity at each pixel can then be calculated. The spatial filter has been used to eliminate the effect of scattering and diffraction of the laser beam propagating through the gap. The two images shown in Figure 3.11 are taken when no high voltage is applied, and the fluctuation patterns in the image without the spatial filter are due to scattering or diffraction of light when propagating through the gap. The distributions of are calculated from the data taken at 0.1 ms (instantaneous voltage Uins~13 kV), which should be uniform across the gap since no significant space charge distortion is present. Obviously, the use of a spatial filter improves the measurement accuracy. Without the spatial filter, the detected gap is wider than reality and the light intensity distribution across the gap has some extra patterns even when there is no high voltage applied. 1500 I1(E)/I1(0) Without Spatial Filter y With Spatial Filter 300 500 100 x x (mm) Figure 3.11. Detected light fields and the distributions of 57 in the gap with and without the spatial filter. The exposure time of the CCD camera (starting from to 2 ms, in steps of 10 μs ( μs) or 50 μs ( ) is adjustable from 50 μs μs). To reduce the random fluctuations in the system (e.g. the variations of laser output intensity), for each the measurement is repeated 50 times and the average of these images is calculated. By differentiating the light intensity under exposure time and between and . Ed/U(t) of the distribution of , we obtain the time average Figure 3.12. Electric field distributions (normalized by U(t)/d) from the measurements with a pair of brass electrodes under 30 kV peak HV impulses of positive polarity. The anode and cathode are at respectively. The scattered point plots are the measurement results at 0 and , 0.3, 0.5, and 0.7 ms. In Figure 3.12, normalized electric field distributions between a pair of brass electrodes under +30 kV peak HV impulses are presented. The measurements are taken at times 0.3, 0.5, and 0.7 ms. The solid lines are polynomial fitting curves, from which one can clearly see the advancement of the space charge fronts as marked by the arrows. The sequence displays the 58 movement of charge carriers across the gap (the mobility of charge carriers is estimated to be ~0.8×10-7 m2/Vs, which is actually the electrohydrodynamic mobility since the turbulent motion of liquid enhances the charge transport by 1~2 orders [3-11]). Therefore the measurement results in the presence of space charge are plausible. The charge injection includes complex electrochemical reactions (e.g. preferential adsorption of ions) controlled by the electrical double layer potential [3-12,3-13,3-14,3-15]. In this case, the anode injects positive charges which drift toward the cathode under the action of the electric field. Near the cathode, the positive ‘charge injection’ is more likely the accumulation of positive charge carriers, since the advancing speed of the charge fronts here is about the same as that at the anode (in transformer oil, the mobility of negative charges is about half that of positive ones [3-3]). In Chapter 4, we will discuss the mechanism of charge injection in more detail. (a) (b) Figure 3.13. Measurement accuracy (a) and fluctuation level (b) as a function of time when the measurements are taken with aluminum electrodes under 30 kV peak HV impulses. 59 To proceed, it remains necessary to experimentally determine a valid time range for Kerr measurements to ensure the accuracy and consistency of the results. In our previous work [3-7], we concluded that when the instantaneous voltage Uins < 10 kV, Kerr measurement results will be heavily contaminated by the random fluctuation of the laser beam (the relative error exceeds No space charge 10%). With space charge Limits given by minimum voltage Upper limit given by the onset of flow Figure 3.14. Determination of the valid time range for the Kerr electro-optic field mapping measurements. On the other hand, as shown in Figure 3.13, the relative error and fluctuation level increase as time increases, implying that there exists an upper time limit (see Figure 3.14). In Figure 3.13, the relative error is defined as the relative difference between the integration of the measued electric field across the gap and the instantaneous applied voltage. The dashed line in Figure 3.13(a) is the tolerated error, 10%. The fluctuation level represents the consistency of the results from the 50 repeated measurements. It is the Euclidean distance between the electric field distribution obtained from each single optical measurement and that 60 from averaged data of 50 optical measurements. The maximum and minimum fluctuation levels at 1, 2, 4, 6, 8, 10, 12, 14, 16, 18 ms are shown in Figure 3.13(b). In Figure 3.13(a), somewhere between 6 ms and 8 ms, the relative error crosses the dashed line. The elevated level of the errors afterwards suggests that a certain physical process has been involved, which is the electrohydrodynamic instability: Coulomb force on space charge in the fluid gives rise to fluid motions. The viscous diffusion time τv= whether fluid inertia with mass density or fluid viscosity determines dominates fluid motions over a characteristic length [3-1,3-4]. If higher spatial resolution is required (smaller ), the onset of significant flow effects will arise earlier. We choose , and τv is on the order of 10 ms. The estimation supports the measurement results that for t < 6 ms there is no strong turbulence, since the relative error is close to the space charge free case (~5%). The main conclusions of this section are summarized in Figure 3.14, which gives the valid time range for the Kerr measurements that can be experimentally determined. There are three basic considerations: (1) magnitude of the electric field to be measured (if it is too low, the Kerr effect signal will be contaminated by the noise); (2) flow effect (flows can bring in strong local fluctuations initially and significantly lower the measurement accuracy eventually); (3) space charge movement (in this work we did not find any limits imposed by space charge, however, keep in mind that the theory of Kerr effect is based on a perfect dielectric material assumption, and it is necessary to examine to what extent can conduction cause deviations from theory). 61 3.4 Results and discussions The procedure of impulse breakdown voltage tests outlined in Section 3.3 are repeated 5 times for each combination of electrodes, and the statistics of the 5 breakdown peak voltages ( ) are presented in Table I. Due to the long pulse duration which reduces pre-breakdown randomness, the standard deviation of breakdown voltages in each test is < 10%. Table 3.3. Impulse breakdown test results for combinations of brass and aluminum electrodes under both polarities. Test # Polarity HV GND Std. (kV) Range (ms) 1 2 +/− +/− Brass Aluminum Brass Aluminum 46.7/47.8 32.6/33.1 2.3/2.1 1.8/2.0 1.21−1.78 0.96−1.37 51.4±3.9 49.1±3.2 3 − Brass 4 + Aluminum Aluminum 33.2 2.1 Brass 33.8 2.8 0.95−1.64 49.6±4.1 5 + Brass Aluminum 52.0 3.3 6 − Aluminum Brass 50.3 2.6 0.20−0.42 50.2±4.5 While the polarity effect on Avg. (kV) (kV) for dissimilar-material electrodes can be clearly seen in Table 3.3 (there is ~50% difference in same-material electrodes (the difference in under opposite polarities), it is not obvious for under two opposite polarities is within the error bounds given by the standard deviation), indicating that the two same-material electrodes are basically identical. Otherwise, if one of them has more micro-protrusions or adsorbed impurities and therefore a much higher probability of breakdown inception, the streamers will tend to develop from this electrode instead of the other. Then the breakdown voltages under the two polarities cannot be so close, since the streamer polarity is reversed under reversed impulse polarity and the inception voltage of positive streamers is significantly lower than that of negative streamers [3-3,3-6]. 62 From the breakdown waveforms recorded by the oscilloscope, the time breakdown occurs (the beginning of the applied waveform is range of when ) can be measured. The for each case is also presented in Table 3.3. In most cases (except in Tests #5&6) the breakdown occurs on the falling slope of the impulse, with ms. Since the time for streamers to transverse the 2 mm gap (in order of nanoseconds [3-5]) is negligible compared with , the streamer is essentially initiated at . The experimental fact that breakdown is initiated after the peak passes implies that the electric field near the electrodes at may be higher than that at the peak, which implies the existence of space charge distortion of the electric field. If it is interpreted as impurity-induced breakdown, there will be difficulties in explaining why almost all breakdown events are later than the impulse peak. To evaluate the intrinsic breakdown strength of the electrodes, we run the breakdown test in a different way. By applying an impulse with peak voltage two times higher than the breakdown voltage obtained using the rising-voltage method, the breakdown will occur on the rising slope of the impulse ( 50 μs) with uniform electric field distribution since no significant space charge effect exists [3-7]. The instantaneous voltage at the breakdown point ( ) is measured, and the statistical results are presented in the rightmost column of Table 3.3. No polarity effect on is observed for all combinations of electrode materials. In the field of dielectric breakdown and electrical insulation research, the term ‘polarity effect’ is most commonly associated with conduction, pre-breakdown and breakdown phenomena in non-homogeneous electric fields (e.g. tip-sphere). As in the ASTM D3300-12 standard, the polarity effect on electrical breakdown under 2.5/50 μs impulse is essentially resulted from different inception field thresholds at the tip and propagation dynamics of 63 positive and negative streamers in the pre-breakdown stage [3-6]. On the other hand, in a space charge free uniform electric field between parallel-plate electrodes, the initiation of streamers can be from either the anode, the cathode, or both. As shown above, if the two electrodes are ‘symmetric’, i.e. made of the same material and with the same surface conditions, or if the effective impulse duration is so short that the electric field is not significantly distorted by the injected charge before streamer inception, no polarity effect on breakdown voltage is expected. Therefore, it is generally thought that the polarity of the applied voltage has little or no effect on the impulse breakdown strength of an insulating medium in homogeneous electric fields [310]. However, in parallel-plate electrode geometry, under longer impulses, the polarity effect on the breakdown voltage for dissimilar-material electrodes has been observed, which may be closely related to charge injection. To reveal this, Kerr electro-optic field mapping measurements will be taken to determine the electric field distribution and its dynamics between parallel-plate electrodes in high voltage pulsed transformer oil. In Figure 3.15, we present the local electric fields at anode and cathode under impulses with 30 kV peak voltage from to ms for 4 combinations of electrode materials: (a) both brass (unipolar positive charge injection); (b) both aluminum (unipolar negative charge injection); (c) aluminum anode and brass cathode (bipolar hetero-charge injection); (d) brass anode and aluminum cathode (bipolar homo-charge injection, with the highest impulse breakdown voltage , see Table. 3.3). In order to reduce the randomness caused by small- scale turbulent flow, the electric fields presented here are the averages of the data at the 25 pixels (0.1d) nearest to the electrode surfaces. The electric fields as a function of time are not very smooth due to measurement error. The dashed lines are the space-charge-free uniform 64 field (Uins/d). The grey shadowed areas mark the ranges of time when breakdown occurs. The charge injection patterns are determined not only by the resulting electric fields at anode and cathode (for example, in unipolar positive charge injection, anode/cathode field is lower/higher than the space charge free field), but also by the evolution of electric field profiles such as those in Figure 3.12. (a) (b) (c) (d) Figure 3.15. Local electric fields at anode and cathode under impulsed with 30 kV peak voltage from to ms for 4 combinations of electrode materials: (a) both brass; (b) both aluminum; (c) aluminum anode and brass cathode; (d) brass anode and aluminum cathode. 65 The peak voltage of impulses used in the Kerr measurements is 30 kV, below the lowest which is ~33 kV for cases (b) and (c). The reason for this is to avoid electrical breakdown when the camera is acquiring data; otherwise, the detected images will be corrupted by bubbles or bright sparks [3-16]. The consistency between the impulse breakdown tests and the Kerr measurements under a lower voltage can be seen from three aspects: (1) In each case, the range of (the grey shadowed area in Figure 3.15) approximately covers the time interval during which the field at one of the electrodes approaches and then passes the ‘crest’, which makes sense because the electrical breakdown is more probable under higher fields. It is understandable that there may be minor discrepancies. On the one hand, and , are measured with higher voltages than that used in Kerr electro-optic measurements. On the other hand, the Kerr measurement results have a ~5% error bounds due to randomness in the system. (2) The intrinsic breakdown voltages ( ) for all electrode combinations are basically at the same level, which serves as a precondition for improved in case (d) from other cases. If of aluminum electrodes is significantly lower than that of brass electrodes, case (a) would have the highest , and in case (d) will most likely be of the aluminum electrode since the breakdown occurs at the peak of the high voltage impulse as shown in Figure 3.15(d). (3) In all cases, cannot exceed (see Table. 3.3), which agrees with physics intuition that space charge is ‘deleterious’ in electrical insulation. Correspondingly, in Figure 3.15, the highest field at one of the electrodes never falls below the peak of the space charge free field (dashed line). In Figure 3.15(d), it is not bipolar homo-charge injection that allows higher , because the breakdown occurs when space charge effects are insignificant. In this sense, the hypothesis should be restated as: 66 in the presence of bipolar homo-charge injection, compared with other charge injections, may be closer to . Similar results are found with stainless steel and brass electrodes. As shown in Table 3.4, with stainless steel electrodes (also injecting negative charges) replacing aluminum electrodes, the difference in the impulse breakdown voltages of various electrode combinations can also be explained by charge injection. Table 3.4. Impulse breakdown test results for combinations of brass and stainless steel (S-S) electrodes. Test # Polarity HV GND 1 2 +/− +/− Brass S-S Brass S-S 3 − Brass 4 + S-S 5 + 6 − Avg. (kV) Std. (kV) Range (ms) (kV) 46.7/47.8 35.4/35.5 2.3/2.1 1.5/1.7 1.21−1.78 1.03−1.55 51.4±3.9 48.8±2.5 S-S 31.6 1.9 Brass 32.1 1.4 0.93−1.47 49.3±3.2 Brass S-S 45.7 2.4 S-S Brass 46.9 2.7 0.25−0.37 49.8±2.9 Although further efforts should be made to test more electrode materials, the present work clarifies some issues regarding the hypothesis at the beginning of the chapter. To test the hypothesis, many experimental details need to be carefully considered, such as appropriate impulse waveform, similar intrinsic breakdown voltage of different electrode materials, and dynamic Kerr measurement before the onset of flow. Only under specific circumstances, the hypothesis is testable and correct. On the other hand, however, this chapter demonstrates the smart use of electrode charge injection to improve the breakdown strength in transformer oil and more importantly, a feasible approach to investigating the effect of electrode material on the breakdown strength, which may be difficult and inconclusive to be directly related to the electronic, mechanical and thermodynamic characteristics of the metal. The complexity has been reduced to charge injection patterns and intrinsic breakdown strength in this work. 67 References [3-1] M. Zahn, Y. Ohki, D. B. Fenneman, R. J. Gripshover, and V. H. Gehman, “Dielectric Properties of Water and Water/Ethylene Glycol Mixtures for Use in Pulsed Power System Design”, Proc. IEEE 74, 1182 (1986). [3-2] M. Zahn, “Optical, Electrical and Electromechanical Measurement Methodologies of Field, Charge and Polarization in Dielectrics”, IEEE Trans. Dielectr. Electr. Insul. 5, 627 (1998). [3-3] I. Adamczewski, Ionization, Conductivity and Breakdown in Dielectric Liquids (Taylor&Francis, London, 1969). [3-4] M. Zahn, “Conduction and Breakdown in Dielectric Liquids”, in Wiley Encyclopedia of Electrical and Electronic Engineering Vol. 20, pp. 89-123 (1999). [3-5] J. G. Hwang, M. Zahn, F. O’Sullivan, L. A. A. Pettersson, O. Hjortstam, and R. Liu, “Effects of Nanoparticle Charging on Streamer Development in Transformer Oil-Based Nanofluids”, J. Appl. Phys. 107, 014310 (2010). [3-6] V. Y. Ushakov, Insulation of High-Voltage Equipment (Springer-Verlag, Berlin, 2004). [3-7] X. Zhang, J. K. Nowocin, and M. Zahn, “Evaluating the Reliability and Sensitivity of the Kerr Electro-Optic Field Mapping Measurements with High-Voltage Pulsed Transformer Oil”, Appl. Phys. Lett. 103, 082903 (2013). [3-8] Q. Liu, Z. D. Wang, and F. Perrot, “Impulse Breakdown Voltages of Ester-Based Transformer Oils Determined by Using Different Test Methods”, in Annual Report of CEIDP, Virginia Beach, USA, pp. 608-612 (2009). [3-9] X. Zhang, J. K. Nowocin, and M. Zahn, “Effects of AC Modulation Frequency and Amplitude on Kerr Electro-Optic Field Mapping Measurements in Transformer Oil”, in Annual Report of CEIDP, Montreal, Canada, pp. 700-704 (2012). [3-10] ASTM, Standard Test Method for Dielectric Breakdown Voltage of Insulating Oils of Petroleum Origin under Impulse Conditions, ASTM Std. D3300-12 (2012). [3-11] N. Felici, “High-Field Conduction in Dielectric Liquids Revisited”, IEEE Trans. Electr. Insul. 20, 233 (1985). [3-12] R. P. Joshi, J. Qian, S. Katsuki, and K. H. Schoenbach, “Electrical Conduction in Water Revisited: Roles of Field-Enhanced Dissociation and Reaction-Based Boundary Condition”, 68 IEEE Trans. Dielectr. Electr. Insul. 10, 225 (2003). [3-13] A. Denat, “Conduction and Breakdown Initiation in Dielectric Liquids”, in Proc. ICDL, Trondheim, Norway, Jun. 26-30, pp. 1-11 (2011). [3-14] T. J. Lewis, “Basic Electrical Processes in Dielectric Liquids”, IEEE Trans. Dielectr. Electr. Insul. 1, 630 (1994). [3-15] R. P. Joshi, J. Qian, K. H. Schoenbach, and E. Schamiloglu, “A Microscopic Analysis for Water Stressed by High Electric Fields in the Pre-Breakdown Regime”, J. Appl. Phys. 96, 3617 (2004). [3-16] X. Lu, Y. Pan, K. Liu, M. Liu, and H. Zhang, “Early Stage of Pulsed Discharge in Water”, Chin. Phys. Lett. 18, 1493 (2001). 69 70 4 Transient charge injection dynamics in high-voltage pulsed transformer oil Synopsis Transient electrode charge injection in high-voltage pulsed transformer oil is studied with Kerr electro-optic measurements. Time evolutions of total injected charges and injection current densities from two stainless-steel electrodes with distinct surface roughness obey a power law with different exponents. Numerical simulation results of the time-dependent drift-diffusion model with the experimentally-determined injection current boundary conditions agree with measurement data. The power-law dependence implies that the electric double layer processes contributing to charge injection are diffusion-limited. Possible mechanisms are proposed based on formative steps of adsorption-reaction-desorption, revealing deep connection between geometrical characteristics of electrode surfaces and fractal-like kinetics of charge injection. 71 4.1 Introduction Non-polar and weakly polar dielectric liquids (e.g. transformer oil) are widely used for high voltage (HV) insulation in electrical power systems. Electrical conduction in these liquids under intense electric fields has been studied for decades [4-1,4-2]. As shown in Figure 4.1, when flow electrification is negligible (e.g. under impulse HV), bulk dissociation and electrode injection are the primary physical processes contributing to the conduction current. Applied Voltage, Gap Configuration electrode processes and impurity effects 1 Liquid Ionization D 1: Integration Law 0 EdxU 2: Gauss’Law dE dx ?: Drift and diffusion of charges, various Electric Field ? 2 Bulk Dissociation Electrode Injection (heterocharge distribution) Space Charge Figure 4.1. The complexity of electric field determination. Given applied voltage and gap configuration, one has to know the interactions between electric field and space charge to solve for electric field. However, quantitative account of the electrode charge injection is difficult. In the bulk of the liquid, the generation and transport of charge carriers have been described by a bipolar drift-diffusion ionic conduction model, two simplified scenarios of 72 which, i.e., steady-state conduction [4-3] and unipolar drift-dominated conduction [4-4,4-5], yielded analytical results. The model assumptions include: (i) Electroquasistatic (EQS) approximation, since the ratio of length and time scales of the system is far less than the speed of light; (ii) Drift-diffusion approximation, i.e. ion motion modeled by drift and diffusion under local field, meaning that the ions immediately relax to a velocity where the field acceleration balances the momentum losses due to collisions with other particles; (iii) Creation of ions (two types, positive and negative) according to Onsager’s theory [4-6], in which the ionic conductivity is due to dissociation of ion pairs and other ionic complexation processes [4-7] are considered insignificant; (iv) Recombination based upon the Langevin model [4-8], which, strictly speaking, is valid for high-pressure gas; (v) Einstein relation [4-9], assuming liquid in thermodynamic equilibrium, builds a connection between diffusion coefficient and mobility for each carrier Electrode charge injection has been included as boundary conditions in the numerical simulation of the time-dependent conduction model, e.g. zero [4-10] or field-proportional [4-11] injected charge densities at the electrode-liquid interfaces. These boundary conditions are largely hypothetical, and the experimental verifications based on steady-state measurements (i.e. ac modulation technique) are unsatisfactory [4-11,4-12]. Current density-electric field (J-E) characteristic is a more naturally defined boundary condition. For example, electronic charge emission from the electrodes can be well described by vacuum electronic models [4-13] (high-field, typically > 73 V/m, requiring highly divergent electric fields such as those at a needle tip). In this work we consider equilibrium and non-equilibrium electric double layer (EDL, thickness much smaller than the inter-electrode distance) phenomena which includes 1D Onsager effect (ions overcome image charge attraction) [4-14] and electrode/liquid interfacial charge transfer electrochemical reactions mediated by EDL. The latter is believed to be the main cause of field-enhanced conduction in highly insulating liquids in homogeneous fields [4-15]. The structure and dynamics of EDL have been a major topic of modern electrochemistry [4-16] and colloid science [4-17]. Treating the dielectric liquid as weak electrolyte, previous works analyzed the steady-state charge injection effects, e.g. field distributions [4-18] and J-E characteristics [4-19,4-20]. As shown in Figure 4.2, a reaction scheme (of impurity molecules) consisting of three formative steps, i.e., adsorption, red-ox reaction, and desorption, has been proposed as a unipolar negative charge injection mechanism [4-19]. EDL Metal Adsorption e- Neutral molecule Liquid Reaction Electric Field Desorption Drift (injection) Figure 4.2. Illustration of the three-step scheme for charge injection: specific adsorption, charge transfer reaction in EDL, desorption. While charge transport is drift-dominated in the bulk of the liquid, the EDL processes injecting charges at the metal-liquid interface are diffusion-limited, which, as will be shown later in this chapter, are closely related to the roughness of electrode surfaces via fractal geometry concepts and models. 74 Quantitative analysis indicates that it works only under long-term HV applications [4-1]. However, under strong dc electric field, in addition to interfacial electrochemical processes, turbulent flow resulted from electrohydrodynamic (EHD) instability [4-21] also affects charge injection [4-7] (like in flow electrification [4-22]). The steady-state analysis may have reflected the combined effects of electrical, thermal and EHD transport observed on a larger time-scale. Therefore, it may be problematic when applying the “steady-state” results to the transient response under short HV impulses with insignificant flow effects. Actually, the difference between transient (~1 ms) and steady-state (> 1 min) charge injection patterns in dielectric liquids has been found as early as in 1960s [4-23]. For electrolyte, the transient injection current density is significantly higher than that in steady state due to smaller thickness of the Nernst diffusion layer [4-16]. It is of interest to examine if similar phenomenon can be found in dielectric liquids with a much lower bulk conductivity under voltages 4~5 orders higher than that applied to electrolyte. On the other hand, understanding transient charge injection under pulsed excitation is important since it is the foundation of a promising approach to improving electrical breakdown strength. Electrical breakdown, as the consequence of sudden increase in applied HV, usually exhibits impulsive voltage characteristics. Charge injection, modifying the electric field near the electrodes, may enhance or inhibit breakdown initiation [4-24]. The smart use of charge injection to improve impulse breakdown strength in transformer oil has been demonstrated in a recent work [4-25], while a systematic study of the time-dependent charge injection dynamics remains in demand. The major difficulty lies with the time-resolved measurements of electric field distribution in transformer oil. In this chapter, Kerr electro-optic measurements with a high sensitivity camera [4-12,4- 75 25] are conducted to map the electric field profile in a transformer oil-filled gap between parallel-plate electrodes. The experimental data will be compared with the simulation results of drift-diffusion conduction model with charge injection boundary conditions. Evidence of fractal kinetics will be presented for transient charge injection, and physical interpretations of the fractal kinetics will be made. 76 4.2 Identification of fractal-like charge injection kinetics The detailed experimental setup of the Kerr measurements including the description of oil conditions and electrode preparation has been introduced in previous chapters and recent papers [4-12,4-26]. The differences made in this work are: (1) The gap spacing between two parallel-plate electrodes is of interest (ROI) is a mm, and the region mm2 rectangle around the center of the gap, corresponding to about pixels in the imaging area of the charge-coupled device (CCD); (2) The rise-time and duration of the single square-wave pulses are respectively 1 µs and 1 ms, and the amplitude is adjustable from 10 to 30 kV; (3) While the HV electrode is made of titanium, there are 2 different grounded stainless steel electrodes: milled with surface roughness µm (I) and electro-polished with µm (II); (4) The measurements are taken by triggering the pulsed laser and the CCD camera at μs to 1 ms, in steps of time 20 μs (the effective exposure time is ~1 ns, the pulse width of the laser). Figures 4.3-4.8 present the measured electric field distributions along a line (as stated above, there are 250 different lines) across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms with 10 kV, 20 kV, and 30 kV HV for both cases (I) and (II). The titanium anode and stainless steel cathode are located at and , respectively. Under each condition, the measurements are repeated 50 times and then the averaged data is used for further processing. 77 Figure 4.3. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 10 kV. Figure 4.4. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 20 kV. 78 Figure 4.5. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (I), 30 kV. Figure 4.6. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 10 kV. 79 Figure 4.7. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 20 kV. Figure 4.8. Kerr electro-optic measurement results of electric field distributions along a line across the gap ( ) at 0.25 ms, 0.5 ms, 0.75 ms, and 1.0 ms: case (II), 30 kV. 80 Consistent with previous results [4-12], the titanium anode at injects an insignificant amount of charges within the time range of the measurements. In Figures 4.3-4.8, the negative slopes of the field distributions near the cathode at indicate unipolar negative charge injection from the stainless steel electrodes. The injected charges will be transported toward the opposite electrode under the action of strong electric field. An interesting observation of Figures 4.5&4.8 is that as the injected charges arrive at the opposite electrode, the significantly increased local electric field may be a precursor of electrical breakdown initiation. According to the Einstein relation, diffusion is much weaker than drift in the bulk of the liquid [4-9]. The mobility of the injected negative charges can be estimated from the propagation speed of the “wave-fronts” in Figures 4.3-4.8, which has to be experimentally determined to use in the numerical model. The propagation speed is approximately the product of the electric field and the mobility. To verify this, at around and 1 ms, the wave fronts are located in Figures 4.3 and Figure 4.4, respectively. We see that as the HV doubles, the propagation speed also increases proportionally. By tracking the advancement of the wave front position (e.g. every 0.1 ms) under each experimental condition and then using linear fitting to find the propagation speed, the negative charge mobility is determined as (4.1±0.4)×10-8 m2/Vs, which is 1-2 orders higher than the previously reported values [43,4-10]. The enhanced mobility may be due to EHD instability [4-27] (to avoid this, low voltages were used to measure the mobility, which looks paradoxical since the dielectric liquids are usually under high-voltage work conditions). Besides, considerable amount of highmobility impurities may be suspended in the transformer oil or adhered to the electrode surface, upgrading the average charge carrier mobility. 81 Our primary goal in this work is to investigate the differences in the charge injection behaviors of the two electrodes with distinct surface roughness. The information presented in Figures 4.3-4.8 is less visually clear for this purpose. Now the total injected charge from unit area on the electrode surface at a given time instant is calculated as follows: Step 1. Find the charge density at each pixel in the gap from the spatial derivative of the electric field distribution (Gauss’ law); Step 2. Integrate the charge densities over the whole gap. The result will be denoted by since it has the dimension of surface charge density. Figures 4.9-4.12 show the total injected charge as a function of time for cases (I) and (II) in linear and log-log coordinates. Figure 4.9. Time evolution of , total injected charge per unit electrode area, plotted in linear coordinates: case (I). 82 Figure 4.10. Time evolution of , total injected charge per unit electrode area, plotted in linear coordinates: case (II). Figure 4.11. Time evolution of , total injected charge per unit electrode area, plotted in log-log coordinates: case (I). The solid lines are the results of linear fitting. 83 Figure 4.12. Time evolution of , total injected charge per unit electrode area, plotted in log-log coordinates: case (II). The solid lines are the results of linear fitting. In spite of the fluctuations resulted from measurement inaccuracy, from Figures 4.9&4.10 one can see that in both cases the temporal evolution of growth rates of is not a linear one. The display a damping tendency as increases. In Figures 4.11&4.12, linear fitting is well made in the log-log coordinate, indicating power law dependence, i.e. where the units of respectively. For case (I), , (20 kV); (10 kV); The coefficient , , and (10 kV); (30 kV). For case (II), (20 kV); , are nC/mm2 and ms, , , (30 kV). is obviously an increasing function of applied voltage . In this work, however, this aspect of charge injection will not be explored due to incomplete information (e.g. chemical composition of the oil and surface layer of the metal) and complexity (e.g. 84 detailed reaction schemes). There are two key observations regarding the exponent : Firstly, for the same electrode, either case (I) or (II), is basically the same under all 3 applied voltages; Secondly, for the rougher electrode surface in case (I), greater than for the smoother electrode surface in case (II). Thus it is concluded that surface roughness plays an important role in transient charge injection dynamics, in addition to physical and chemical properties of electrode and dielectric materials, oxidation layer and defects on metal surface, impurity composition in the liquid and on the surface, applied voltages, surface treatments, etc. It is reasonable to assume that the space charge and current in the bulk of the liquid are due to electrode injection (the simulations of previous work [4-10] and ours show that without charge injection, negligible space charge effect appears in tens of milliseconds). Therefore the charge injection current density is approximately ; for case (II), (absolute value). For case (I), . This time-explicit form of charge injection is called fractal or fractal-like kinetics [4-28,4-29]. 85 4.3 Numerical simulations of drift-diffusion conduction model In 1D Cartesian coordinates with independent variables x and t, the governing equations are [4-10,4-11]: (4.1) (4.2) (4.3) where Equation (4.1) is the equation for bipolar drift-diffusion current density; Equation (4.2) is the continuity equation for time-dependent charge transportgeneration-recombination; Equation (4.3) is Poisson’s equation; ( ) is positive (negative) charge density; ( ) is current density in and direction due to transport of positive (negative) ions; are electric potential and field; is the permittivity (for our transformer oil F/m); are ion mobilities (from previous work [4-3], the positive charge carrier mobility , while has been experimentally determined in Section 4.2); are diffusion coefficients (the Einstein relation [4-9] gives: is the Boltzmann constant, is absolute temperature and 86 is the charge per ion); , where stands for the rate of charge recombination (according to Langevin model [4-8], with the recombination coefficient ); stands for the rate of charge generation (ion-pair dissociation). the dissociation constant and where is is the concentration of ion pairs. In the absence of applied HV, the dielectric is assumed to be in thermal equilibrium (all symbols with the subscript ‘0’) with uniform charge distribution , which is related to the Ohmic conductivity . Under this condition, the neutrality of the liquid requires that by and . Field-enhanced dissociation constant takes the form of (Onsager’s theory [4-6]), where is the Bessel function of the first kind and order one, and . The values of the above-mentioned physical parameters are: the lowvoltage equilibrium Ohmic conductivity S/m, room temperature and by considering the simplest (also most probable) dissociation case , where C is the elementary charge. The Equations (4.1)-(4.2) can be transformed to the following advection-diffusionreaction form: (4.4) (4.5) To implement the model Equations (4.4), (4.5) and (4.3), continuous variables such as and are sampled with uniform time step electrodes there are kth time step ( cells inside which ). 87 and spatial step and ( , that is, between the ) are defined at the The initial conditions ( ) are , . At the (k+1)th time step, the charge densities are updated according to Equations (4.4)&(4.5). Then Equation (4.3) is solved again to update the electric potential distribution under boundary conditions . With and , we can compute the updated current densities and electric field, and then move forward to the next time step. The numerical algorithm has two parts: a) Solution of Equation (4.3) to with first-type boundary conditions A compact finite difference method [4-30] is used to calculate the spatial derivatives (for simplicity, below means the spatial derivative of at th cell, or the local electric field with opposite sign): The first order derivatives can be given at interior cells ( ) using a 6th-order tri-diagonal scheme: (4.6) At boundary cells , the 3rd-order formula is as follows: (4.7) (4.8) , the 4th-order formula is as follows: At boundary cells (4.9) For the second order derivatives, we just need to replace equations with s and s and s in the above s. b) Solution of Equations (4.4)&(4.5) to with charge injection boundary conditions The transport equations for positive and negative charges are discretized using the 88 Crank-Nicolson method [4-31], which is second-order implicit in time, and numerically stable. It transforms each component of the equations into the following: (4.10) (4.11) (4.12) We can now write the scheme as: (4.13) where , , At boundary cells . , charge injection boundary conditions are used: (4.14) (4.15) (4.16) (4.17) where , as determined experimentally in Section 4.2. As shown in Figure 4.13, a drawback of the Crank-Nicolson method is that it responds to jump discontinuities in the initial conditions with oscillations which are weakly damped and therefore may persist for a long time [4-32]. To reduce the spatial error oscillations, the 89 implicit Euler scheme is used for the first several simulation time steps, in which Equations (4.11)&(4.12) take the form: (4.18) (4.19) 36 36 0.25 ms 0.25 ms 0.75 ms 34 34 32 32 E (kV/mm) E (kV/mm) 0.75 ms 30 30 28 28 26 26 24 24 0 20 40 60 80 100 120 140 160 180 200 0 Spatial steps 20 40 60 80 100 120 140 160 180 200 Spatial steps (a) (b) Figure 4.13. Numerical solutions of electric field distribution under 30 kV applied voltage at 0.25 ms and 0.75 ms. The number of spatial steps is 200; the number of time steps is 2000. (a) Crank-Nicolson; (b) The CrankNicolson with implicit Euler for the first 10 time steps. The numerical solutions of the local electric fields near anode and cathode surfaces are shown in Figures 4.14-4.17. The experimental results are also presented for comparison. The error bars come from the statistics of measurement data on 250 different lines in the ROI (along the electrode surfaces). The simulation results of the drift-diffusion model agree quantitatively with the experiments (note that Kerr electro-optic measurements have a relative error of 3%~5%). 90 Figure 4.14. Numerical solutions of the local electric fields near anode and cathode surfaces: case (I), anode. Figure 4.15. Numerical solutions of the local electric fields near anode and cathode surfaces: case (I), cathode. 91 Figure 4.16. Numerical solutions of the local electric fields near anode and cathode surfaces: case (II), anode. Figure 4.17. Numerical solutions of the local electric fields near anode and cathode surfaces: case (II), cathode. 92 As fast transient response to step excitation, the unique feature of the phenomenon in insulating liquid compared with that in electrolyte is that the current injection at the electrodes has a non-local effect, i.e. injected charges will be transported to the bulk of the liquid in a drift-dominated manner and distort the electric field distribution over the whole gap. For unipolar negative charge injection, the electric field at the cathode is reduced. However, as the transient injection current dampens, this tendency may slow down or even slightly reversed (the 30 kV cases in Figures 4.15&4.17). 93 4.4 Discussions What is the nature of the injection current? The direct (electronic) charge transfer from the electrode to the oil requires higher electric field, even after taking into consideration the field enhancement factor (~10) due to micro-protrusions. So cathode electron emission cannot be the primary source of the injected charges. Instead, the injection should be ionic. As illustrated in Figure 4.2, the simplest physical picture of the origin of injection current is that neutral species like impurity molecule is specifically adsorbed to electrode/liquid interface and undergoes reduction (accepting electrons) in the EDL. Then the product is removed from the interface by desorption and transported into the bulk by electrical force. The power-law dependence of current density on time indicates that the surface reaction is diffusion-limited, which may be resulted from: (1) a much lower adsorption rate than reaction rate; (2) anomalous lateral diffusion of reacting molecules. Correspondingly, there are two possible interpretations of the fractal-like charge injection kinetics. For (1), the adsorption-limited current density is given by: (4.20) where is the fractal dimension (FD) of the medium [4-29,4-33]. In this work, the medium is the part of EDL (of typical thickness 1 nm) where the reaction takes place. For an ideally smooth electrode surface, in-plane homogeneity of EDL can be assumed. very close to the result of case (II) above. In case (I), , , , which seems counterintuitive since the FD of a rough surface is generally greater than two [4-34]. 94 , Figure 4.18. Mechanisms for fractal-like charge injection kinetics. (a) If the surface reaction is adsorption-limited, on rougher surfaces, the protrusions are dominant in adsorbing neutral molecules (D is the diffusion constant, t is the duration of HV pulses), while on smoother surfaces, the pores also make significant contributions. (b) If the surface reaction rate is controlled by lateral diffusion of reacting molecules, anomalous diffusion along fractal surface may account for the origin of fractal charge injection kinetics. To resolve this, we find that the active EDL contributing to injection current may cover only part of the electrode surface (e.g. like the Sierpinski carpet with a FD of 1.89). In Figure 4.18(a), the rough electrode surface is represented by an array of protrusions and pores. If the reaction is adsorption-limited, for very rough surfaces, the effective adsorption region around a protrusion is much larger than that inside the pores. The majority of injection charges originate from the protrusions. The parts of EDL near all protrusions on the electrode surface form a fractal structure with . If adsorption is a fast process compared to reaction or the supply of adsorbed molecules is sufficient, the current density of a reaction-limited process would be time-independent. In order to understand the fractal-like kinetics, one need to take into account the sub-diffusion due to the heterogeneous (fractal) interface structure that slow down the random walk of reacting 95 agents [4-35,4-36], which yields a current density proportional to reaction rate: (4.21) where is the FD of the whole EDL, diffusion, is the anomalous diffusion exponent. For normal , i.e. the mean-square distance of a random walker is proportional to In case (II), assuming that the EDL can be regarded as a smooth surface, , corresponding to a “well-mixed” homogeneous reaction. For case (I), sub-diffusion , it follows that . , . Since for , a general feature of rough surfaces. In this chapter, the fractal-like charge injection kinetics in HV pulsed transformer oil has been identified from Kerr electro-optic measurement data and verified by numerical simulations of the time-dependent drift-diffusion model with the experimentally-determined injection current boundary conditions. It is demonstrated that while the space charge process in the liquid bulk is drift-dominated, the charge injection kinetics from the EDL on the electrode-dielectric interface is diffusion-limited. We propose two mechanisms to reveal the deep connection between geometrical characteristics of electrode surfaces and fractal-like kinetics of charge injection. The order of injection current densities is 10-5~10-3 mA/mm2 in our experiment, corresponding to total current of about 10-2~1 mA in the gap and bulk conductivity enhanced by 104~106. With such a large magnitude, it seems that the transient charge injection should be associated with the charging dynamics of EDL. Otherwise, the formative steps in Figure 4.2 would be the same as in previous studies which work only under long-term HV applications [4-1,4-19]. 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Freeman, San Francisco, 1983). [4-35] D. Ben-Avraham and S. Havlin, Diffusion and Reactions in Fractals and Disordered Systems (Cambridge University Press, New York, 2000). [4-36] H. Sakaguchi and R. Baba, “Charging Dynamics of the Electric Double Layer in Porous Media”, Phys. Rev. E 76, 011501 (2007). 99 100 5 Electro-optic signal fluctuations as indicator of critical transitions in dielectric liquids Synopsis Motivated by the search for approaches to non-destructive breakdown test and inclusion detection in dielectric liquids, we explore the possibility of early warning of breakdown initiation in high voltage pulsed transformer oil from the data of Kerr electro-optic measurements. It is found that the light intensities near the rough surfaces of electrodes both fluctuate in repeated measurements and vary spatially in a single measurement. We show that the major cause is electrostriction which brings disturbances into optical detection. The calculated spatial variation has a strong nonlinear dependence on the applied voltage, which generates a precursory indicator of the critical transitions. 101 5.1 Introduction The behavior of dielectric materials under strong electric fields determines critical transitions in insulation systems, i.e. the initiation and development of partial or full dielectric breakdown. When an insulating liquid is stressed by a high voltage impulse, without breakdown, there are three major phenomena involved: (1) Electrostriction (a modification of pressure distribution due to changes in the liquid density) [5-1]. (2) Conduction (including molecular ionization and recombination, electrode-liquid interfacial processes, and transport of charge carriers) [5-2,5-3]. (3) Electro-hydrodynamic (EHD) flow (as we discussed in Chapter 3, its onset time is scale dependent) [5-4]. Besides, the presence of inclusions (bubbles and particles adhered to the electrodes and suspended in the liquid) further complicates the problem [5-5,5-6]. In previous chapters, we mainly discussed the electric field distribution influenced by space charge due to conduction or charge injection. We now consider electrostriction (this chapter) and EHD flow (flow). On the one hand, their presence is a major source of error and fluctuation in the electric field measurement. On the other hand, these phenomena themselves are of great theoretical and practical interests. If the applied high voltage pulse duration is very short (sub-microsecond), the conduction dynamics and flow effects may be weak, and pre-breakdown streamers can be initiated in the absence of substantial ionization in the bulk of the liquid [5-7,5-8]. Electrostriction becomes the dominant driving force of pre-breakdown phenomena. Under this 102 condition, the following discharge initiation mechanism looks plausible [5-9,5-10,5-11]: as the electric field exceeds a threshold, electrostriction shock waves may be excited, giving rise to voids/bubbles that will ionize to form the initial discharge channel. This physical picture has its implications in the non-destructive detection of gaseous/metallic inclusions in dielectric liquids. In general, the electric field near inclusions in the liquid is greatly increased [5-12], resulting in a greater likelihood of electrical breakdown [5-5,5-9]. The electrostriction effects under short impulses become more significant due to higher local electric field and increased inhomogeneity of the medium [5-1,5-10,5-11]. Locating the enhanced electrostriction spots with an applied voltage below the threshold for partial discharge initiation may be a promising approach for inclusion detection. To capture the electrostriction effects in dielectric liquids, previous works [5-1,5-10,5-11] have used highly-divergent electrode geometries (e.g. needle-plate) to make sure that the discharge is initiated at the needle tip where the initial phase of breakdown can be observed via Schlieren transmission imaging (as refractive index varies spatially in transparent liquid). Binary in nature, Schlieren imaging is possible only when the voids/bubbles have grown large enough, which obviously has limited sensitivity under lower electric fields and unavoidably causes destructive effects due to subsequent breakdown. In this chapter, we will study parallel-plate electrode configurations in the most widelyused insulating liquid, transformer oil. Compared with the needle-plate geometry in which almost all detectable phenomena appear near the needle tip, the use of parallel-plate electrodes, with a quasi-uniform background, can provide a higher “contrast” necessary for the detection of local electric field enhancement around inclusions or near electrode surfaces. In parallelplate geometry, however, more sensitive optical measurement techniques are needed, since the 103 maximum electric field is much lower than that in highly-divergent geometries with the same gap spacing stressed by the same voltage. The Kerr electro-optic measurement with a high-sensitivity charge-coupled device (CCD) [5-13,5-14,5-15,5-16,5-17,5-18] will be used for our purpose. The image of the electrostriction pattern may be difficult to acquire, because this effect is much weaker than the Kerr effect and the electrostriction dynamics has great uncertainty. Nevertheless, an electrostriction wave induces non-uniform liquid density distribution, which affects the optical detection and may be identified via statistical data processing. Enhanced electrostriction effects also exist in the case of electrical breakdown initiation near the electrode surface, which, with no need for carefully prepared oil samples with controlled inclusions, will first be tested in this work as preliminary verification of the principle. By measuring the electrostriction near the electrode surfaces, it may also enrich the conceptual framework for the transition to electrical breakdown as the applied voltage is increased. An interesting analogy is the laminar-to-turbulent transition in fluid dynamics [519,5-20,5-21]. When a control parameter of the system (e.g. Reynolds number) becomes large enough, the transition takes place. Flows in the transitional regime display laminar-turbulent intermittency, which resembles the statistical behavior of electrical pre-breakdown phenomena (e.g. may or may not result in breakdown). Furthermore, the effectiveness of passive control techniques to delay the transition has been demonstrated for fluid flows [5-22], while smart use of electrode charge injection is shown possible to improve the breakdown strength [5-18]. From an even broader perspective, this work attempts to extend recent research on early warning signals for critical transitions in complex dynamical systems [5-23]. Generic indicators predicting the catastrophic shifts (tipping points) are found in slowly-evolving 104 systems, such as population [5-24,5-25,5-26,5-27], climate [5-28], and environmental [5-29] dynamics. A review of some related concepts will be presented in Section 5.2. While electrical breakdown is a certain type of critical transition in dielectric liquids with its time scale in the microsecond to nanosecond range [5-9], little attention has been paid to exploring the idea of electrical breakdown as a critical transition with predictive indicators. Apparently, this is because the process of electrical breakdown is so rapid and violent, characterized by a fast growing current. However, most measurements in dielectric liquids have been made at electrical terminals of voltage and current, providing no information on electric field distribution in the bulk, which is important in breakdown initiation and can be measured by using Kerr electro-optic techniques In this chapter, statistical analysis of the Kerr measurement data will show that spatial variance can be a predictive indicator of breakdown in advance of detectable current increase. The potential applications include an estimation of breakdown voltage without breakdown. Usually breakdown tests need to be done to evaluate the breakdown strength of a material. If there do exist early warning signals for breakdown, non-destructive breakdown tests will be made possible, and as a result some insulation failures may be avoided or have reduced damage. 105 5.2 Indicators of critical transitions in complex systems In many complex systems, there are catastrophic thresholds called tipping points across which the system states experience a sudden shift to distinct regimes. These systems range from ecosystems and the climate to financial markets and the society. It is of great importance to predict such critical transitions, though this could be extremely difficult. This is because as the tipping point approaches, experimentally the state of the system may just change unnoticeably, and theoretically the model of the system may not work reliably due to approximations made. For electrical breakdown in dielectrics, the above features also exist. In this context, the critical threshold corresponds to breakdown voltage, and the critical transition is breakdown (insulating state to conducting state). Figure 5.1 shows typical voltage (a) and corresponding current (b) waveforms when a pair of parallel-plate stainless-steel electrodes are stressed by 1 µs (rise-time) /1 ms (duration) high voltage pulses. The voltage is measured by a capacitive divider, while the current is measured at the high voltage side with a Rogowski coil. As the applied peak voltage is increased, the probability of electrical breakdown rises from 0 (case III) to 1 (case I). The sign of loss of “resilience” means that the insulation becomes increasingly vulnerable to voltage instabilities (perturbations). The initial fluctuations seen in the current waveform in Figure 5.1(b) should be displacement currents interacting with inductive elements in the electrical system. In case II, once breakdown is initiated, the magnitude of conduction current increases by 5-6 orders in less than 10 ns, which captures the feature of abrupt (catastrophic) change of state in critical transitions of complex systems. 106 Figure 5.1. Typical voltage (a) and corresponding current (b) waveforms when a pair of stainless steel electrodes are stressed by 1 µs/1 ms high voltage pulses. 107 The possibility of using generic statistical early warning signals to indicate if a critical transition is approaching has been studied extensively. There are generally two categories of predictive indicators: temporal and spatial. The former is primarily based on a phenomenon known in dynamical systems theory as “critical slowing down”, i.e. slow recovery from small perturbations in the vicinity of tipping points. The latter, usually extracting particular spatial pattern for systems consisting of many coupled units distributed in space, is less generic than the former and requires details of each system. The symptoms of critical slowing down include increase in autocorrelation and fluctuation. As the system approaches critical point, the time it takes to recover from small perturbations will be longer and therefore the system may become more correlated with its past. This increase in “memory” can be measured by looking at the autocorrelation of the time series of the system dynamics. The larger variance or fluctuation is another possible consequence of critical slowing down. Intuitively, this is the accumulating effect of perturbations since they decay slowly. Other statistical indicators such as skewness and flickering before transitions have also been demonstrated, which, however, do not result from critical slowing down. Early warning of catastrophic transitions based on critical slowing down may correspond to a fold (catastrophic) bifurcation in the system dynamics, though it also exists for other classes of bifurcations. Figure 5.2(a) shows the modeled response of semi-arid vegetation to increasing dryness of the climate. Solid/dashed lines are stable/unstable equilibrium points. Close to the transition point, a small perturbation is able to drive the system from the upper (vegetated) to the lower (barren) branch. Figure 5.2(b) is the conceptual counterpart in impulse dielectric breakdown, in which the phase shift may be either through a catastrophic bifurcation or across a non-catastrophic threshold. 108 (a) 1 0 Large change Breakdown Probability Catastrophic bifurcation Non-catastrophic threshold Small forcing Applied Voltage (b) Figure 5.2. (a) Bifurcation diagram of a model desert vegetation system undergoing predictable sequence of spatial patterns as approaching a critical transition (from [5-23], which was modified from [5-29]). (b) The breakdown probability as a “function” of applied voltage. Catastrophic bifurcation may or may not exist. In either case small forcing (i.e. increase in voltage) will lead to a distinct state. 109 The width of the transition zone shown in Figure 5.2(b) is typically several kilovolts, relatively small compared to the absolute value of breakdown voltage. The dashed line represents unstable “fixed points”, which is unobservable using standard breakdown test methods. Instead, in high voltage engineering, it is usually assumed that the dependence of impulse breakdown probability on the applied voltage takes the form of a non-catastrophic threshold process. However, this does not indicate the impossibility of the catastrophic bifurcation. In breakdown tests, due to the stochastic nature of the process, the change in breakdown probability cannot be fine-tuned in a predictable manner by adjusting the applied voltage. Considerations on sample quality and test cost also prevent us from doing the tests too many times. Hence the number of measurable breakdown probabilities is always limited. For example, we may know the voltages corresponding to 50% and 90% breakdown probabilities. But the details in between remain unclear. Catastrophic bifurcation may exist. While the studies in time series ignore spatial interactions for real systems, spatial patterns as early warning signals are much richer. For some systems, critical transitions are preceded by the appearance of particular spatial patterns or the change of spatial configurations in a predictable way. The insets in Figure 5.2(a) are some spatial patterns: the dark color represents vegetation and the light color represents empty soil. The transition of the ecosystem to a barren state can be predicted by the change of the patterns from maze-like to spots. Sometimes spatial data are more accessible. This has different meanings in relatively slow population dynamics and very rapid electrical breakdown process. For the former, generally long-term observations are necessary to obtain the predictive power of temporal warning signals. For the latter, when we take Kerr measurements with very short high voltage pulses, the maximum frame rate of the camera usually allows very limited numbers (in the case 110 of our high-sensitivity high-resolution CCD camera, it's only one) of images, resulting in poor time resolution. For our applications, we will mainly discuss spatial indicators. The two reasons are given below: Firstly, the dielectric liquid between two electrodes cannot be assumed to be the same everywhere without spatial coupling. For example, the liquid near the electrode surface is stressed by higher electric fields due to the existence of electric double layer. And different parts in the liquid are interconnected by transport processes. Secondly, the temporal data is ineffective in generating any early warning signal of the approaching critical transitions. In case II of Figure 5.1(a), with peak voltage ranging from 31 to 39 kV, statistically speaking, the higher the voltage is, the higher the breakdown probability ( ) will be. There is also a time difference ( ) between 1 µs and the instant when breakdown occurs. The random nature of electrical breakdown is no-good for non-destructive inclusion detection and breakdown test. The next option, the current shown in Figure 5.1(b), does not prove to be more useful. The measured conduction currents ( ) are indistinguishable from noise in both case (II) before breakdown and case (III), since the conductivity of transformer oil is very low ( ). In the absence of measurement techniques or instruments with exceedingly higher sensitivity, monitoring conduction currents cannot provide predictive indicators of electrical breakdown. 111 5.3 Electro-optic precursor of breakdown initiation in transformer oil The detailed experimental setup of the Kerr measurements has been introduced in Chapter 2. The description of oil conditions and electrode preparation can be found in Chapter 3. The differences made in this chapter are: (1) The gap spacing between two parallel-plate electrodes is mm; (2) The duration of the high voltage pulses is 1 ms while the rise time is adjustable from 100 µs to 10 ns; (3) The grounded stainless steel electrode is unpolished with surface roughness µm, while on the high voltage side, the electrode is electro-polished with µm. In recent reports [5-17,5-18] on Kerr electro-optic measurements with high voltage pulsed transformer oil, to reduce the fluctuation due to uncertainty and randomness in the system, under each experimental condition, multiple images are taken and then averaged. In order to improve measurement sensitivity, we should identify and correct various errors in the system. For this purpose, the statistical analysis of the measurement data is necessary. The detected light intensities both vary from pixel to pixel in a single measurement and fluctuate at each pixel in repeated measurements. In principle, a laser beam with quasi-uniform intensity distribution is needed to illuminate the 1 mm gap. Usually one can use a beam expander to expand part of the laser beam to achieve this goal. However, as shown in Figure 5.3(a), the expanded beam propagates through the gap as if it is in a waveguide. Extra pattern (bright and dark lines like interference pattern) is generated, possibly due to the light bouncing back and forth between the two electrodes. The edges of the gap become blurred due to 112 scattering and diffraction effect. One solution is to move the CCD to several meters away from the test cell, which eliminates the pattern but meanwhile sacrifices the detection sensitivity. High-voltage electrode y (j) 1 mm x (i) Grounded electrode (a) (b) Figure 5.3. (a) The image of the gap illuminated by an expanded laser beam. (b) The background light intensity distribution in the gap leaked from crossed polarizers as the 1 mm gap is illuminated by a Gaussian beam (7.6 mm in diameter). The region of interest (ROI) is recorded in a 120-by-60 (row-by-column) matrix. Therefore we just use the original Gaussian beam from the pulsed laser. Figure 5.3(b) shows the light intensity distribution without applied voltage, in which a rectangular area is chosen as the region of interest (ROI). We use a matrix to record the light intensity distribution in ROI, which has 60 pixels in the y (or j) direction (along the electrode surface) and 128 pixels in the x (or i) direction (across the gap). The location of electrode surfaces in the x direction has a 2~4 pixel error, so 4 rows of data both on top and bottom of the original matrix have been discarded (now ). We first study the shot-to-shot optical signal fluctuation caused by laser beam scintillation, scattering near the electrode surfaces, and even the influence of high voltage pulse on the laser and the CCD. Figure 5.4(a) presents the distribution of the fluctuations 113 (normalized by the averages) of the measured pixel light intensities in 1,000 repeated measurements. The influence of room light has been minimized (<0.5%) by reducing the exposure time of the CCD to 10 µs (the actual exposure time, however, is about 1 ns, the duration of the laser pulse) and increasing the laser output power. (a) Std./Ave. 0.07 0.06 0.05 0.04 0.03 40 j (b) Std./Ave. 0.06 0.07 0.065 0.06 0.06 0.05 0.055 0.05 0.04 20 0 0 40 0.05 60 0.045 80 j i 30 0 0 40 80 i Figure 5.4. The distributions of fluctuations (normalized by the averages) of the measured pixel light intensities in multiple measurements. (a) with no high voltage pulse generated, at most pixels, the standard deviations of the light intensities in the 1,000 measurements stay below 5% of the averaged light intensities; (b) with high voltage pulses firing nearby, there is no substantial difference in the fluctuation level compared with (a), indicating that electromagnetic compatibility is adequate for our measurement system. Without any applied voltage across the 1 mm gap, optical signal fluctuation level is due to laser beam scintillation (output power fluctuation and propagation in media with stochasticity) and possibly the internal errors of the CCD. Since the fluctuation level at the boundaries is similar to that in the mid-gap, it may be concluded that the effect of random scattering at electrode surfaces is insignificant. In Figure 5.5(b), the histograms and fitted normal distributions of the light intensities at two pixels (#1 and #2 marked in Figure 5.5(a), which is the same as Figure 5.4(a)) are 114 High-voltage electrode 1 mm presented. The mid-gap (#1) light intensity is about 10% higher x (i) than that near the electrode surface (#2). However, we are only interested in the fluctuation level (ratio of standard y (j) deviation and average). Grounded electrode (b) Std./Ave. 0.06 0.07 0.06 0.05 0.05 #2 0.04 #1 0.03 0.04 40 j Probability Density (×10−3) (a) 1.2 1.0 0.8 0.6 0.4 0.2 80 20 0 40 0 i (c) (d) Figure 5.5. (a) Same as Figure 5.4(a). With no applied voltage, the standard deviations of the light intensities at most pixels in the 1,000 measurements stay around 5% of the averaged light intensities. (b) The histograms and fitted normal distributions of the light intensities at two pixels, #1 and #2 marked in (a). Further, still no applied voltage across the transformer oil gap in the test cell, we apply high voltage pulses to an air gap (covered with black cloth in order not to send any light to the optical system) placed close to the test cell (without blocking the light path). When the air gap discharges, a strong current will spread in the conducting surface of our optical bench on which the laser and the CCD sit. Besides, every time the Marx generator fires, high frequency interferences couple into the power cord of both instruments, bringing in additional instability of their performances. We insert plastic sheets under the laser and the CCD to insulate them from the optical 115 bench, and use isolation transformers as power supplies for all electronic instruments in the measurement systems. Consequently, the optical signal fluctuation level has been cut from 10% to 5% (as shown in Figure 5.4(b)), i.e., no substantial difference from Figure 5.4(a), indicating that electromagnetic compatibility is adequate for our measurement system. Hence any upgraded fluctuation level at a pixel (defined as the ratio of standard deviation and average of detected light intensities in multiple measurements) with high voltage applied to the oil gap should be attributed to field induced effects, like electrostriction and EHD flow. We conduct Kerr measurements under 10 ns/1 ms, 1 µs/1 ms, and 100 µs/1 ms pulses with positive peak voltages of 10 kV, 20 kV, 25 kV, and 30 kV. For Kerr measurements the results of which will be presented in Figures 5.6 8, the images are taken at beginning of the high voltage pulses as time (setting the ). That is, all the images are taken at approximately the voltage peak. In each row of the matrix , we first compute the fluctuation level at each pixel in 1,000 repeated measurements, and then find the average of the fluctuation levels of all pixels in the row. Results of 3 rows with (cathode surface), (mid-gap), and (anode surface), are shown and compared in Figs. 5.6(a) (c). It is found that, while the fluctuation levels are generally higher under higher applied voltages, which can be attributed to field induced effects, like electrostriction and EHD flow, the upgrading rate of the fluctuation level depends both on position and pulse. Generally, close to the rougher cathode surface, the increase in the fluctuation level is faster than other positions in the gap. And for longer rise time pulse, the fluctuation is stronger. 116 (a) (b) y j from 1 to 60 Cathode x i from 1 to 120 Anode (c) (d) Figure 5.6. The average fluctuations in row i=1(cathode), 60(mid-gap), and 120(anode) at various stantaneous voltages with rise-time of the pulses being (a) 100 µs, (b) 1 µs, and (c) 10 ns. (d) is an illustration of matrix , which is used to store the pixel light intensity distribution in the ROI. Figure 5.7 presents the distributions of average fluctuation levels across the gap for three cases with the same voltage (+30 kV) but different rise times from 10 ns to 100 µs. The pixels with strongest fluctuations (>10%) are marked in the insets. We choose not to take images after 117 100 µs delay to minimize the space charge behavior and large-scale EHD turbulence [3-16]. The results of the Kerr electro-optic field mapping in all three cases, based on the averages of detected light intensities, are close to a uniform field distribution with acceptable measurement errors (two types of errors have been defined in Chapter 2). Now, however, we have two interesting observations about the distribution of the strongest fluctuations. Firstly, the cathode surface is rougher than the anode surface, which means that the local electric field enhancement due to micro-protrusions on the cathode is more significant than that on the anode. As a result, both electrostriction and EHD flow, though still unable to tell which one is the major process, will be stronger near the cathode surface, creating more disturbances and uncertainties in the light intensity measurement (random scattering due to surface roughness may be a secondary effect also contributing to fluctuations). This explains why the fluctuations are more intense on the cathode side. Secondly, strongest fluctuation spots seem more localized to (certain parts of) electrode surfaces as the rise time of the high voltage pulses decreases. Keep in mind that the rise time of the pulse is also the time when Kerr measurements are taken. By adjusting the rise time from 100 µs to 10 ns, the fluctuation level in the middle of the gap is lowered. The size of a pixel in our CCD camera is about 8×8 µm2. Based on the estimation of viscous diffusion time [5-18], the time for the onset of EHD instability over a pixel size is in the order of 10 µs. This smallscale turbulence may increase the fluctuations in optical measurements. On the other hand, sub-microsecond pulses are preferred for the generation and detection of electrostriction waves since these transient patterns tend to damp and diffuse due to relaxation and dissipation over longer course. For µs and 10 ns, it may be concluded that the strongest fluctuations near the two electrode surfaces are primarily due to electrostriction. If the rise time is even shorter 118 (and meanwhile the high voltage impulse generator and other instruments can still work reliably and accurately), with negligible EHD effect and preserved electrostriction, we may even be able to locate those spots on the electrodes from which, statistically speaking, electrical breakdown will be initiated. Figure 5.7. For 3 cases with about the same instantaneous voltage (+30 kV) but different rise times from 10 ns to 100 µs, the distributions of average fluctuations across the gap are shown, and the pixels with strongest fluctuations (>10%) are marked. Figures 5.6&5.7 give us a hint that certain measure of the enhanced shot-to-shot fluctuations (most likely near the cathode surface) under higher voltages may be an electro- 119 optic precursor of electrical breakdown. However, 1,000 repetitive Kerr measurements will become less possible since accidental breakdown occurs more frequently as the applied voltage is getting closer the breakdown voltage (the 50% breakdown voltage is 35~36 kV, and 30 kV is in fact the highest voltage that we have succeeded without breakdown). Breakdown is unwanted during Kerr measurements because it till take us a long time to reset the test cell and more importantly, it causes damage to the imaging parts of the CCD. Instead, we will examine the light intensity distribution from a single Kerr measurement to identify a more practical (and economic) warning indicator. The highest voltage for single Kerr measurements reaches 32 kV (by taking advantage of the relatively low breakdown probability). Figure 5.8. The slice-by-slice image entropy distributions with zero and 30 kV applied voltages. 120 The amount of information in an image can be quantified as entropy, a statistical measure of randomness characterizing the “texture” of the image [5-30]. We cut the ROI into 12 slices (each consisting of rows from to , where slice number and use the MATLAB function to find the image entropy ), for each slice. The results with zero and 30 kV high voltages are Figure 5.8, which confirms our intuition that an early warning signal of electrical breakdown is more likely to be found near the rougher cathode surface. Figure 5.9. The coefficient of spatial variance of the cathode slice as a function of applied voltage. The error bars are drawn based on the data from multiple measurements. 121 If we assume the pixel light intensities within a slice are subject to normal distribution with mean ( and variance (analogous to Fig. 5.5(b)), it can be estimated [5-31] that , or . According to this, the variance of the cathode slice and ) grows by about 50% as the applied voltage is increased from 0 to 30 kV. In Figure 5.9, we use the coefficient of variation, , to describe the spatial fluctuations in the optical measurement data. The value of the coefficient of spatial variance is ~3% when there is no applied voltage. The error bars in Figure 5.9 are drawn based on the results from multiple measurements. When the voltage is over 30 kV, the error is more significant partly because only 5~10 measurements have been made for each case. As shown in Figure 5.9, spatial variance rises slowly when the voltage is lower than 30 kV; as the breakdown voltage is approached, there is a significant acceleration in the increase of spatial variance (at 32 kV which is 90% of the 50% breakdown voltage, the coefficient of variance jumps over 10%, which can be viewed as an indicator of the vicinity of electrical breakdown). Electrostriction, interacting with gaseous and solid impurities activated by high field, may be the underlying mechanism. However, a detailed analysis of these processes involved is out of scope of the present work. 122 5.4 Discussions Previous sections explore the possibility of early warning of electrical breakdown initiation in high voltage pulsed transformer oil from the data of Kerr electro-optic measurements. Due to electrostriction, the detected light intensities near the rough surfaces of electrodes both fluctuate in repeated measurements and vary from pixel to pixel in a single measurement. The calculated coefficient of variation has a strong nonlinear dependence on the applied voltage, implying that some critical transitions are taking place, at least at some spots on the electrodes. The results of this work may be helpful to develop new approaches to nondestructive breakdown test and, based on the same physical principle, non-destructive inclusion detection in dielectric liquids. As mentioned in Section 5.2, in dynamical systems theory, critical slowing down (slow recovery from small perturbations in the vicinity of transition) has been suggested as the leading indicator of whether the system is getting close to a critical threshold. As shown in Figure 5.10, some phenomenon similar to critical slowing down near transitions in complex systems has been found. (It has to be pointed out that the analogy regards the high voltage pulse as some kind of perturbation to the dielectric liquid, which is not true. Strictly speaking, the voltage fluctuation seen in the waveform of the pulse corresponds to perturbation in dynamical systems theory.) After the 1 ms pulse has passed, there is essentially no applied voltage across the gap. However, the detected light intensity will not fall back to the zero field value immediately as expected by the Kerr measurement principle [5-17]. The transition time scale (milliseconds) is far beyond any dielectric relaxation process (<nanosecond). On the other hand, as confirmed by our tests without any applied voltage, flow caused by transient 123 temperature/pressure gradient can only increase the fluctuation level in the detected light intensity, and cannot increase the mean value of the detected light intensity. The phenomenon shown in Figure 5.10 may be associated with some kind of relaxation process, the details of which remain unclear. It might be an interesting topic for continuing research. Figure 5.10. A phenomenon similar to critical slowing down. (a) The 1 ms square wave pulse and the ratio of the detected light intensity and the zero field value. All light intensities have been averaged over the ROI. (b) For 10, 20, 30 kV pulses, the time it takes for the light intensity to drop to the zero field value is approximately 1, 3, 10 ms, respectively. 124 The initiation and development of partial or full dielectric breakdown remain not fully understood. Work in this area can be divided into two classes: experiments on breakdown characteristics and numerical simulation of streamer dynamics. Neither of them can be easily connected to the physical theory of critical phenomena. This, however, does not necessarily mean impossibility. Our work exploring the possibility, though inspired by researches in other fields, is based on statistical processing of the measurement data. The image shown in Figure 5.11 was taken by fast imaging technique in the early stage of breakdown development (the full, destructive breakdown is unavoidable). It agrees with our results in Figure 5.7 that electric field enhancement takes place at localized sites on the electrode surface. The difference is, our methods with much higher optical detection sensitivity do not rely on the appearance of visible discharge plasma channel and can predict how close it is to the breakdown without actually reaching this point. Figure 5.11. (From [5-32]) Localized discharges (streamers) on cathode on uniform electric field. The gap spacing is 4 mm. The liquid is n-hexane. The image was taken about 1 µs before breakdown. Figure 5.12 shows the typical chronogram of interference bands registered under voltage pulses with an amplitude of 120 kV applied to extended electrodes in de-ionized water (slit 125 scanning, which means the horizontal axis in the image represents time while the top and bottom dark areas are occupied by electrodes). The electrostrictive excitation originates from the electrode surface (the formation of the wave pattern is mainly due to the repetitive application of pulses). This may also viewed as a “collateral evidence” of our work, in which we interpret the cause of the optical detection fluctuation as enhanced electrostriction. Figure 5.12. (From [5-9], page 17) Experiment on electrostriction wave excitation in water in the system of extended electrodes (slit scanning). Additional work needs to be done to find more evidence that electrostriction is the major force behind the early warning signal. The influence of a strong electric field on a liquid is noticeable when the electric field energy density is comparable with the external pressure [5-9]. This condition is usually satisfied in the case of breakdown initiation. We can place the test cell inside a pressure chamber with a wide range of adjustable pressure. Theoretically, it is expected that the critical threshold of the applied voltage would be higher under higher pressures. Under the same applied voltage, the detected fluctuation in electro-optic signal should strongly depend on the ambient pressure. 126 The influences of applied voltage (peak, rise time, polarity), electrode material and surface roughness, and ambient pressure on the electrostriction effects need also be investigated. In the field of dielectric and electrical insulation research, the most common impulses are microsecond instead of nanosecond. We will start from nanosecond rise-time pulses and gradually increase the rise-time to the microsecond range. By doing this it is possible to find a characteristic time beyond which the space charge behavior dominates. Since parallel-plate electrodes are used, we do not expect any polarity effect if the two electrodes are ‘identical’. This can be a basic check of the reliability of the measurement results and the processed data. Finally we would like to propose experimental procedure on the non-destructive inclusion detection. Prepare transformer oil with conductive inclusions of nm to µm diameter range. The first type is a dilute nanofluid; the second type is to release a small number of conducting micrometer-size suspensions between the two electrodes. Test transformer oil samples with these controlled conducting inclusions to measure the resulting local electric field enhancement which can be a trigger for electrical breakdown or partial discharge. This method can easily be extended to larger scale industrial systems by scanning the entire liquid region. 127 References [5-1] M. N. Shneider and M. Pekker, “Dielectric Fluid in Inhomogeneous Pulses Electric Field”, Phys. Rev. E 87, 043004 (2013). [5-2] A. Denat, “Conduction and Breakdown Initiation in Dielectric Liquids”, in Proc. ICDL, Trondheim, Norway, Jun. 26-30, pp. 1-11 (2011). [5-3] T. J. Lewis, “Basic Electrical Processes in Dielectric Liquids”, IEEE Trans. Dielectr. Electr. Insul. 1, 630 (1994). [5-4] A. 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Conf. on Conduction and Breakdown in Dielectric Liquids, Delft University Press, pp. 49-54 (1975). 130 6 Electro-optic signatures of turbulent electroconvection in dielectric liquids under dc and ac high voltages Synopsis In this chapter, signatures of turbulent electroconvection in transformer oil stressed by dc and ac voltages are identified from Kerr electro-optic measurement data. It is found that when the applied dc voltage is high enough, compared with the results in the absence of high voltage, the optical scintillation index and image entropy exhibit substantial enhancement and reduction respectively, which are interpreted as temporal and spatial signatures of turbulence. Under lowfrequency ac high voltages, spectral and correlation analyses also indicate that there exist interacting flow and charge processes in the gap. This chapter also clarifies some fundamental issues on Kerr measurements. 131 6.1 Introduction Electroconvection refers to the flow motion due to injected ionic charges under applied electric field, which plays an important role in the electrical conduction phenomena in dielectric liquids [6-1]. It is of practical interests in a wide range of applications such as electrostatic spraying [6-2], electrostatic precipitator [6-3], and even random number generation [6-4]. The theoretical framework for understanding the onset of electrohydrodynamic instabilities has been established since the 1970s [6-5, 6-6, 6-7], implying the ubiquity of electroconvective turbulence in electrical insulation systems (the working voltages are always much higher than the threshold of instability). Recent numerical studies of the problem in two [6-8, 6-9] and three [6-10] spatial dimensions have also shown the existence of turbulent motions as well as ordered patterns in electroconvection. On the other hand, due to the necessity of keeping the liquid chemically stable and pure to avoid premature electrical breakdown in the presence of high electric fields [6-6, 6-7], quantitative flow measurement techniques [6-11, 6-12] are generally not applicable to turbulent electroconvection. Schlieren visualization was only able to provide some qualitative results [66]; it remains unclear to which extent they can be compared with theoretical results. Kerr electro-optic technique was used to map the electric field distribution in high voltage (HV) stressed liquid dielectrics [6-7], but the measurement principle [6-13, 6-14] simply neglects the effect of flow on the detected light intensities. This is, however, a valid approximation only when signal-to-noise ratio (SNR) is large. In low Kerr constant liquids like transformer oil where high sensitivity photo-detectors are required to record weak electro-optic signals, SNR becomes close to unity. In recent works [6-15, 6-16], to reduce the noise level, multiple 132 measurements are taken and then averaged under each experimental condition. The limitation of this approach is the loss of information carried by the noise that may be associated with specific types of noise sources. In this chapter, we attempt to identify signatures of electroconvective turbulence from the data of Kerr electro-optic measurements with transformer oil and to find experimental conditions under which the negative effect of turbulence on optical detection is statistically insignificant. The two seemingly contradictory goals are actually converging; they are just the two sides of the same problem. Once one is achieved, clues to the other would also be seen. 133 6.2 Spatiotemporal statistical analysis of Kerr electrooptic signal under dc voltages The experimental setup has been introduced in Chapter 2. The main difference is that we no longer use pulsed HV to reduce flow effect. Instead, we use a HV amplifier as the excitation source. The output dc voltages or ac amplitudes are adjustable from 0 to 20 kV. The two parallel-plate electrodes are made of stainless steel with polished surfaces and rounded edges. As shown in Figure 6.1, the region of interest (ROI) is chosen at the center of the transformer oil-filled gap in view of that optical detection near the electrode surfaces may bring in additional uncertainty from diffraction and random scattering due to surface roughness. The ROI corresponds to an array of 128×128 pixels in the imaging area of the high sensitivity charge-coupled device (CCD). Figure 6.2 presents the detected light intensity (unit: electron counts) at a pixel within ROI when there is no applied HV (the liquid is assumed to be at rest, though slight vibrations of the test cell are unavoidable). A total of 500 samples are taken at 5 Hz sampling rate. This is done by synchronizing the pulsed laser Q-switch and the CCD camera exposure with a pulse train at 5 Hz repetitive rate. As the “inherent” output instability of the pulsed laser, the light intensity fluctuates from sample to sample. The approximately symmetric distribution of the detected light intensity is well fitted by both normal and lognormal functions, which means that the disturbance to the light intensity can be modeled as an unbiased additive noise. 134 Window of the Test Cell Light Propagation Laser Beam Profile Electrode (HV) 0 d=2 mm ROI Electrode (GND) CCD Imaging Area x Transformer Oil Figure 6.1. The view as looking into the window of the test cell. The diameter of the pulsed laser beam is 7.6 mm. The imaging area (8×8 mm2) of the CCD camera has an array of 1002×1004 pixels. The width of the gap between two parallel-plate electrodes is d=2 mm, corresponding to about 250 pixels. The 1×1 mm2 region of interest (ROI) is chosen around the center of the gap. × 8000 6000 PDF 0 20 40 60 80 100 Time (s) Light Intensity Figure 6.2. Histogram (bar plot, 500 samples, 5 Hz sampling rate), normal fitting (solid line), and lognormal fitting (dashed line) of the distribution of detected light intensities without high voltage (HV) application. The inset shows the light intensity fluctuations in time. 135 On the other hand, it is well-known that lognormal distribution is the statistical characteristic of the short exposure irradiance (the effective exposure time in our measurements is ~10 ns, the laser pulse duration) of optical scintillation, i.e. electromagnetic wave propagation in turbulent atmosphere [6-17, 6-18]. If under certain HV the detected light intensities display lognormal distribution with substantial deviation from normal distribution, the existence of scintillation effects may be inferred. 200 150 100 2000 10000 50 2000 5000 S Skewness 100 8 kV 18 kV S (c) Voltage (kV) Figure 6.3. The skewness of the detected light intensity distribution as a function of applied HV. The error bars come from statistics at various pixels in ROI. The three regions partitioned by the two dashed lines indicate that the data is very likely skewed positively (above), negatively (below), and inconclusively (middle). The two insets of histograms of light intensities show the slightly (8 kV) and strongly (18 kV) positively-skewed distributions. 136 We then apply dc HV to the gap for about 10 min and then trigger the CCD to acquire sample images (it has been demonstrated [6-19] that the electromagnetic compatibility of our current setup is adequate for our purpose, i.e. the application of HV has no obvious interference with the performance of the laser and the CCD). In Figure 6.3, the skewness of the detected light intensity distribution as a function of applied HV is plotted. The error bars come from statistics at various pixels in ROI. The skewness tends to rise with increasing HV (the absolute value of skewness higher than 0.5 means moderately or highly skewed distributions; otherwise it is called approximately symmetric [6-20]). The two dashed lines in Figure 6.3 indicate the critical values of the test statistic [6-21] (approximately ), i.e. the data is very likely skewed positively (top), negatively (bottom), and inconclusively (middle). From the above statistical analysis it can be concluded that as the applied HV exceeds 8 kV, the distributions of detected light intensity are positively-skewed. Two examples with slightly (8 kV) and strongly (18 kV) positively-skewed distributions are shown. For extremely positively-skewed data, exponential distribution is usually considered [6-17]. In general, for positively skewed data, lognormal distribution is a much better fitting than normal distribution, implying that the signal has a weak multiplicative noise component [6-22]. In our case, the only possible source of this kind of noise is optical scintillation due to turbulent flow of the transformer oil in the gap. At each pixel, the scintillation index of the detected light intensity is defined as the normalized variance [6-23]: , where is the average over all samples. Scintillation index, quantitatively characterizing turbulence-induced scintillation effects, is sometimes considered as a simple indicator of the strength of the turbulence [6-17, 6-23]. 137 (d) S Electro-optical Current (µA) S Optical Voltage (kV) Figure 6.4. The dependence of scintillation index (S) and conduction current on applied HV. In the top plot of Figure 6.4, the significantly increased when HV is in the range of 15- 20 kV can be viewed as the signature of electroconvective turbulence in the gap. By removing the analyzer from Kerr electro-optic measurement setup and adjust laser output accordingly to avoid saturate the CCD, we repeat the above steps and calculate the scintillation index without electro-optic modulation. Similar trend is found (the middle plot of Figure 6.4), but the values of are about 50% lower, which means lower sensitivity. This can be understood as follows: besides optical scintillation, turbulence has an additional effect in Kerr electro-optic measurements. The direction of the HV field is randomly disturbed due to the existence of electroconvective turbulence, which affects the local electric polarization and electrobirefringence of the liquid. 138 The bottom plot of Figure 6.4 presents the conduction currents measured at the HV terminal, relatively low and with an approximately linear dependence on the applied HV. Only with current-voltage relation, one might regard the liquid between the two electrodes as a stationary ohmic conductor, which is not true since the non-polar transformer oil is subject to weak charge injection (to be discussed later in this section) and electroconvective turbulence. For highly insulating dielectric liquids, measurement of terminal currents may not be able to provide useful information on the physical processes in the liquids. Note that our experimental setup does not have enough sensitivity and reliability to accurately determine the onset of turbulent electroconvection; but we are able to reveal the existence of turbulent electroconvection in the gap under high enough applied voltages (e.g. the 18 kV and 20 kV cases) via statistical analysis of temporal sequence of detected light intensities. In fact, the same conclusion can be reached if one takes a closer look at the spatial randomness of single ROI images (spatial sequences) under various voltages. A statistical measure of spatial randomness characterizing the “texture” or the amount of information of an image is Shannon entropy [6-24]: , where is the probability of light intensity occurring in the image. There is a MATLAB function calculating for each image [6-25]. To make the images taken under different voltages comparable, before calculating image entropy, all the images are normalized so that the average light intensity over all pixels is the same value (e.g. 1000). The solid curve in Figure 6.5 shows the ROI image entropy divided by (the entropy in the absence of HV) versus applied HV. At first glance, it seems surprising and counterintuitive that as the voltage exceeds 10 kV, the decrease in 139 begins. However, the loss of entropy is in accord with the physical picture of turbulent cascade which increases the spatial correlations [6-26, 6-27]. The output beam of the pulsed laser has a Gaussian profile. Consequently, the probability distribution of in ROI is approximately normal when the random disturbance field is unbiased with maximum information content [6-28]. Under higher voltage, however, the increased spatial correlation in the turbulent flow field may lead to a biased disturbance field with lower degree of spatial randomness (decrease in entropy). This behavior of image entropy, though distinct from temporal statistics of scintillation index, can also be viewed as a signature H/H0 of electroconvective turbulence. Voltage (kV) Figure 6.5. ROI image entropy (normalized by H0, the value in the absence of HV) versus applied HV under 3 different experimental conditions. 140 The dashed curve in Figure 6.5 is the case with 4-by-4 binning (i.e., reducing the spatial resolution by a factor of 4 in each dimension), in which the decrease of is “postponed”. While this is actually a loss in sensitivity, it also implies that binning of multiple pixels may be able to reduce the effect of turbulence on optical detection. Figure 6.6 shows the scintillation index S evaluated with L-by-L binning (i.e., the average light intensity in a square region containing L× L pixels). The voltage is 20 KV. The dashed line indicates the scintillation level corresponding to about 10% measurement uncertainty, which requres a minimum L of 64 (in this case, there will be only 4 data points over the whole gap). The bar plot in Figure 6.7 presents the Kerr electro-optic field mapping S results. log2L Figure 6.6. The scintillation index S evaluated with L-by-L binning (i.e., the statistics is based on the average light intensity in a square region containing L× L pixels). The dashed line indicates the scintillation level corresponding to about 10% detection uncertainty. The applied HV is 20 kV. 141 E (×10 kV/mm) Texp = 10 ms; L = 1 Texp = 10 ns; L = 64 x/d Figure 6.7. Results of Kerr electro-optic field mapping measurements under 2 different experimental conditions, both of which are heterocharge configuration with enhanced electric fields near the electrodes. The applied HV is 20 kV. Figure 6.8. The scintillation index S evaluated with various exposure times. The dashed line indicates the scintillation level corresponding to about 10% detection uncertainty. The applied HV is 20 kV. 142 Back to laser beam scintillation, the long-exposure beam is approximately diffractionlimited with a smooth Gaussian profile [6-17], which indicates the possibility of reducing scintillation level by increasing the exposure time laser with an adjustable pulse width laser ( . To verify this, we replace the pulsed from 10 µs to infinity). Longer exposure yields similar results as binning, as shown in Figure 6.5 and Figure 6.8. Result of Kerr electro-optic field mapping measurements with ms is presented in Figure 6.7, showing the heterocharge distribution with enhanced electric fields near the electrodes [6-13, 6-29]. The non-dimensional injection parameter [6-1] can now be estimated at the cathode ( ): most previous researches [6-6, 6-7, 6-8, 6-9] . It is a very low level of injection, while in was in the order of 1~10. Even when the charge injection is very weak, with sufficient spatiotemporal resolution it is possible to identify the signatures of electroconvective turbulence. Conversely, the negative effect of turbulence on electro-optic measurements can be mitigated by adjusting the resolution. 143 6.3 Spectral analysis of Kerr electro-optic signal under low-frequency ac voltages The spectral signature of turbulent electroconvection has been found from electrical current measurements three decades ago [6-30]. One of the limitations of our CCD is that its maximum sampling rate is about 100 Hz, which is too low for broadband spectrum analysis of detected light intensities. As a compromise, we apply very low frequency sinusoidal ac HV to Light Intensity Gap the gap and use Fourier transform to analyze the spectral content of the detected light intensity. 1 2' 2 Number of Samples Figure 6.9. Detected light intensities at two pixels labeled 1 and 2 (100 pixels or 0.8 mm apart) when the applied HV is sinusoidal with amplitude 20 kV and frequency fac=0.1 Hz. The sampling rate is 63.53 Hz. A sample image is presented in the inset, in which the bright band actually bounces between the two electrodes at frequency fac. 144 Figure 6.9 shows the detected light intensities at two pixels labeled 1 and 2 (100 pixels or 0.8 mm apart) with HV amplitude 20 kV and frequency fac=0.1 Hz. The sampling rate is 63.53 Hz. Pre-semi polariscope [6-31] with crossed polarizers is used. A sample image is presented in the inset of Figure 6.9, in which the bright band bounces back-and-forth between the two electrodes. Pixel #2 P(f) Pixel #1 Figure 6.10. Fourier spectra magnitude versus frequency at pixels 1 and 2. The dashed lines are the spectra in the absence of HV. If the brighter area means higher electric field, then this motion implies an oscillatory transport of charges in the gap since the gradient in electric field is proportional to the local 145 space charge density (Gauss’ law). In fact, as shown below, the flow driven by the ac HV may play a more important role. From the principle of Kerr measurement [6-13, 6-31], if there is no turbulent flow or unstationary charge distribution in the transformer oil, the only significant harmonic component is at 2fac. However, the data presented in Figure 6.9 obviously have much richer frequency contents. Their different Fourier spectra magnitude versus frequency at pixels 1 and 2 are shown in Figure 6.10. At pixel 1, the primary Fourier component is 2fac while the same frequency component at pixel 2 is a local minima. Additionally, at pixel 2, there seems to be a significant enhancement of subharmonic components. These phenomena cannot be understood within the framework of Kerr electro-optic measurement principle. The spectral evidence suggests that there be interacting flow and charge processes in the gap. Figure 6.11 shows the coefficient of correlation between the time series of light intensities at pixels 1 and 2 (2’) as a function of applied HV amplitude. Even under 20kV (amplitude) ac HV, the data of pixels 1 and 2 are not highly positively-correlated. But there are two general trends: firstly, due to smaller distance apart, 1-2’ has higher correlation coefficient than 1-2; secondly, in both cases, under voltages in the range of 15~20 kV, the data sets become increasingly positively correlated, which may be attributed to eddies of various length scales developed in electroconvective turbulence. It is an interesting observation that the results presented in Figure 6.11 are consistent with Figure 6.5, where the reduced spatial randomness under higher voltages was interpreted as increased spatial correlation due to turbulence. Here we give an example demonstrating the assumption made in the previous section. 146 Correlation Coefficient Voltage (kV) Figure 6.11. The coefficient of correlation between the time series of light intensities at pixels 1 and 2 (2’, which is 10 pixels away from 1) as a function of applied HV amplitude. P(f) 2fac Component f/fac Figure 6.12. Fourier spectra magnitude versus frequency at pixel 1 with HV amplitude 20 kV and 3 different fac values. The sampling rate is 80 Hz. 147 The effect of fac on the Fourier spectra can be seen in Figure 6.12. The sampling rate now is 80 Hz. While only 0.1 Hz and 10 Hz cases have definitive 2fac components, each spectrum has a main lobe, i.e. “plateau” in low-frequency range ( upper frequency limit of the main lobe reaches frequency limit of the main lobe is Hz). For fac=0.1 Hz, the , while for fac=10 Hz, the upper . This implies that, the upper frequency limit is not determined by the ac HV; it should be a property of the liquid itself. The viscous diffusion time [6-32] τv= mass density or fluid viscosity determines whether fluid inertia with dominates fluid motions over gap width . This corresponds to ~10 Hz as the upper frequency limit of the flow effect. The frequency spectrum in the main lobe is in fact the combined outcome of flow and electro-optic effects. For Hz, the component lies outside of the main lobe, the negative influence of electroconvection can be reduced. This conclusion is consistent with our study on the Kerr electro-optic measurement technique called ac modulation, which will be discussed in the next section. 148 6.4 Discussions In this chapter, we have carried out experimental studies to find temporal, spatial, spectral, and correlation electro-optic signatures of turbulent electroconvection in transformer oil stressed by dc and ac HV. The implications of this work are two-folded. Combining theoretical models of optical wave propagation in turbulent medium and statistical characteristics of simulated electroconvective turbulence fields, it might be possible to test and verify numerical results with experimental data. Moreover, this work also clarified some important issues on Kerr electro-optic measurements. The results presented in Section 6.2 refreshed the understanding of the term “steady state” in dielectric liquids stressed by HV, which is meaningful only in statistically averaging sense. The last section demonstrated that to reduce the influence of flow on the optical detection of harmonic components, the modulation frequency should be high enough; and the lower ac amplitude is also desirable. In this section, some elaboration of the second aspect is to be made, which is related to a technique called ac modulation for Kerr electro-optic measurements with low Kerr constant liquids like transformer oil [6-33, 6-34]. In this method, the frequency of the ac voltage superposed on the dc voltage should be high enough so that the ac field does not disturb the space charge behavior in one cycle. And the modulation voltage amplitude, compared with dc level, should not be too high. Qualitativly, the requirements of ac modulation method and the basic conclusions of the previous sections are convergent. To further verify this point, we conduct a preliminary examination of how high (low) the frequency (amplitude) necessary to ensure the measurement accuracy which is missing in published works. 149 Figure 6.13. Illustration of experimental setup for Kerr electro-optic field mapping measurements with ac modulation. The experimental setup consists of two main subsystems, optical and electrical. A test cell with transformer oil and a pair of parallel-plate copper electrodes (alloy 110, surface unpolished) inside is the intersection of the two subsystems. Vacuum pump and filter system are used to remove suspended bubbles and particles in the oil, which prevents premature electrical breakdown and improves optical detection accuracy. There are laser, beam expander, polarizers (P0, P, A), quarter-wave plate (Q), slit and photodiode in the optical subsystem. The intensity-stabilized He-Ne laser is made by Melles Griot, model 05-STP-901. The diameter of the output beam is 0.5 mm with wavelength of 632.8 nm, average power 1 mW and linearly polarized. It takes about 15 min for the laser to lock so that the output light intensity is stable. Any sort of reflection from optical components back into the laser head should be prevented. The 20× beam expander is made by Special Optics. It expands the beam diameter to ~1 cm. 150 The pre-semi circular polariscope configuration is used, as shown in Figure 6.13. The three polarizers are made by Spindler&Hoyer with extinction ratio 500:1 and diameter of 10 cm. P0 is used to attenuate the light to prevent saturation of the photo detector. The output light intensity of P0 is denoted by . The angle of the transmission axis of P is at 45° with respect to the x-axis and that of A (analyzer) is −45° (crossed polarizers). A quarter-wave plate (Q) is inserted between P and the test cell and its slow axis is along the x-axis. The photodiode is made by United Detector Technology, Model UDT-455HS. The bias voltage is 15 V and the detection area is 2 mm by 2 mm. Since the gap between the electrodes is fixed at 2 mm in width, a 2/3 mm movable slit was used to get spatial resolution, which means that only 1/3 of the detection area is active for measurement. The light intensity incident on the slit ( ) is a function of electric field across the gap (and also a function of x). To reduce the influence of room light, the whole system was covered with a black cloth. The output of the photodiode is connected to the lock-in amplifier and the oscilloscope to measure ac (first and second harmonics) and dc components. In the electrical subsystem, the Hewlett Packard function generator, model 3311A, generates both ac and dc signals as inputs of the high voltage amplifier. The high voltage amplifier is made by Trek Inc., model 20/20, which amplifies the combined ac and dc signal by 2000 times in magnitude. The maximum input voltage is 10 V. The output HV is connected to the feed-through on the top of the test cell. A 1000:1 Fluke high-voltage probe and 5000:1 Pearson capacitive divider was used to measure the high voltage. The attenuated signal is connected to the oscilloscope to monitor the applied voltage and to the lock-in amplifier as a reference signal. The lock-in amplifier is EG&G, Model 5210. The time constant is set to 30 seconds for high accuracy and stability of the output. 151 Some constants in the measurement are given below: Kerr constant of transformer oil m/V2, the electrode length along the light path (z-axis) gap width , and the . The electric field in the gap (in x direction) is polariscope with a small Kerr constant ( . For the pre-semi ), the 1st order of is: (6.1) Hence, , (6.2) or equivalently, , (6.3) The dc high voltage applied across the gap is measured by the oscilloscope (with divider) and denoted by frequency . The ac high voltage . The mean ( ) and harmonics ( (peak-to-peak) is at modulation ) of the output of the photo detector can be read from the oscilloscope and the lock-in amplifier display, respectively. Then from Equation (6.3), both the dc and ac electric fields are calculated. The slit can be moved to take measurements at ( in this case) different positions across the gap: H (near the surface of the HV electrode), M (in the middle of the gap), and G (near the surface of the grounded electrode). It should be noted that the spatial resolution in the measurements with a photodiode is relatively low, and H, M and G are not ‘points’. The light intensity 152 detected at H, M or G actually represents the average level in a 2/3 mm interval determined from the slit width. Thus the calculated electric field is also the average value in the each 2/3 mm interval. Measurements under various dc voltages, modulation frequencies and ac amplitudes are taken. Certain criteria are needed to verify the reliability of the results. Firstly, the ac electric field across the gap should be uniform. If not, there would be space charge responding to the ac field and fluctuating at the same frequency, while in the ac modulation method, the ac field is not assumed to significantly disturb the space charge distribution. So the peak ac field everywhere in the gap should be close to the mean peak ac field given by: (6.4) and a good experimental condition minimizes the deviation: (6.5) where the sum is over all measured points in the gap. After obtaining the dc field distribution, it is checked by taking the difference between the integration of dc field across the gap and the applied voltage: (6.6) to determine if it is within an acceptable error range (e.g. 5%). 153 2.5 ΔEac/ Eac(m) (%) |ΔUdc|/ Udc (%) 5 4 3 2 1 2 1.5 1 0.5 0 0 10 1 10 1 2 100 f (H 100 2 3 1k z) f (H 53 10k 4 10 2 50 1 Vp U p/ 53 4 10k 102 50 1 Vp (a) Udc=1kV 10 6 (%) 8 4 2 6 4 2 0 0 F F 10 1 10 1 2 100 f (H z) 2 100 54 1k 3 10 3 4 10k 20 2 50 1 V pp/ Ud f (H %) c( 54 31k z) 3 10 4 10k 2 20 50 1 (b) Udc=5kV 6 Ud V pp/ %) c( 40 ΔEac/ Eac(m) (%) |ΔUdc|/ Udc (%) U dc p/ 10 8 ΔEac/ Eac(m) (%) |ΔUdc|/ Udc (%) 1k 3 z) (%) dc 4 2 30 20 10 F 0 F 10 1 0 F 2 100 f (H z) F F F 10 1 100 2 34 3 1k 53 4 10k 10 2 V pp/ 1 20 ( U dc f (H %) 34 1k 3 z) 53 4 10k 10 2 V pp/ 20 1 (c) Udc=10kV U (%) dc 15 ΔEac/ Eac(m) (%) |ΔUdc|/ Udc (%) 10 10 5 F F 0 F F z) 4 2 F F F F F 10 1 100 2 f (H 6 0 F 10 1 8 100 2 31k 33 4 10k 52 10 1 U dc V pp/ f (H (%) z) 31k 33 10k 4 (d) Udc=18kV Figure 6.14. Errors in measured dc and ac electric fields with dc voltage kV and various modulation voltages ( ) and frequencies ( ). 154 52 10 1 (a) V pp/ U (%) dc kV; (b) kV; (c) kV; (d) Starting with 50%, 10% and 5% of kV, the peak-to-peak values of the ac voltage ( ) are set to be . The corresponding ac amplitudes are 250 V, 50 V and 25 V. The modulation frequency varies from 10 Hz to 10 kHz. There may be difference in values of different points due to the nonuniformity of the background light field . But at at a fixed point can be regarded as a constant when changing modulation parameters, as a result of the stable output of the laser and the irrelevance of to the applied voltage (approximately). From Equations (6.5) and (6.6), the errors in measured dc and ac electric fields are computed, as shown in Figure 6.14(a). One can see that when kV all the errors are less than 5%, which indicates that, when the dc voltage is low, there exists a wide range of modulation frequencies and amplitudes that make the measurement results reliable. Due to the insignificance of the space charge effect at this low voltage, even the modulation frequency as low as 10 Hz and ac peak-to-peak value comparable to the dc voltage yield data of high accuracy. The measurements and calculations were repeated as the dc voltage was increased to 5 kV, 10kV and 18 kV. The errors in dc and ac electric fields are presented in Figure 6.14(b)-(d). There is a new feature in these cases of higher dc voltages, as marked by ‘F’ in Figure 6.14(b)(d). This means the failure of the lock-in amplifier to generate a stable output even over a long period or a correct output with a reasonable order-of-magnitude. Although the causes for the failure are unclear in detail, it is inferred that the response and feedback of space charge to an ac electric field may play a destructive role in the establishment of a ‘steady state’ with a set of relatively stable frequency components. The failures always occur with low modulation frequencies and relatively high ratio of ac and dc voltages. To avoid failures, the modulation frequency should be increased or the 155 applied ac voltage be as low as possible. In addition, the errors also tend to decrease. For example, in Figure 6.14(c), when 10 kV and , the measurements are not successful for modulation frequencies of 10 or 100 Hz. The modulation frequency can either be increased to 1 kHz or the ac amplitude reduced to get stable and reasonable output of the lock-in amplifier. The former results in a great fluctuation in the ac field profile ( over 40%), which is supposed to be uniform over the gap. It is concluded that is not suitable for the measurement due to significant errors. To increase the accuracy and reliability of the measurements the modulation frequency is increased and the applied ac voltage is made as small as possible. If the results are ‘filtered’ by the criterion of both less than 5%, then a range of ‘valid’ modulation frequencies and and amplitudes for each can be determined, which is presented in Figure 6.15. In general, there is an increasingly strict confinement on the applicable range of modulation frequencies and voltages with the increase of . Vpp/ Udc (%) Udc=5kV 20 Udc=10kV 10 5 3 0 Udc=18kV 10 100 1k 10k Figure 6.15. Reasonable ranges of ac modulation frequencies and amplitudes for each f (Hz) 5 kV, 10 kV and 18 kV. For , the reasonable range is the set of the parameter pairs at the same side of the corresponding curve as the arrow. 156 There is a practical implication of the above results. If one wants to replace the photodiode with a modern computerized CCD camera to increase the spatial resolution and the efficiency of data acquisition and processing, the restrictions in the frequency and amplitude of the ac modulation voltage impose requirements on the maximum sampling rate (time resolution), sensitivity and saturation level of the CCD camera. Typically the modulation frequency is chosen to be several kHz, and correspondingly, the order of the average ac field would be 0.1 kV/mm. According to the sampling theorem, in order to detect a double frequency component, the sampling rate needs to be greater than four times the modulation frequency. So the CCD camera should be high-speed, capable to take frames per second. When a CCD camera is used to record a series of output light intensities with no high voltage applied across the gap, a Fourier transform can be done to analyze the frequency spectrum of the background light field. The typical ratio of the measurement magnitudes of double frequency component and dc component is , which requires that, in the background light spectrum, the same ratio should be much lower. Sensitivity, closely related to frequency component magnitude in the background, means the minimum distinguishable signal over the noise level, while saturation level, corresponding to dc component in the background, means the maximum detectable light intensity. Consideration and test of these two parameters are necessary as well as the specification of time and spatial resolutions. In the calculations, the Kerr constant of transformer oil was assumed as m/V2. Since this parameter is crucial in determining the accuracy of the results, a verification of this parameter is done. The dc electric field distributions under various dc high voltages with modulation parameters check, it was assumed 10 kHz and 0.5 kV are measured. As a basic kV/mm, and from Equation (6.2), the results 157 show that holds for every point in all cases. Then back into Equation (6.2), regarding and were substituted as an unknown variable. The final solution is m2/V2, which coincides with what was used in the measurements. E1.4 dcd/Udc 1.2 1 0.8 系列1 H 0.6 系列2 M 系列3 G 0.4 0.2 0 1 Udc=1kV 2 3kV 3 5kV 4 8kV 5 10kV 6 12kV 7 15kV 8 18kV Figure 6.16. Normalized dc electric field distribution between copper electrodes in transformer oil under various dc voltages ( ) measured with ac modulation 10 kHz and 0.5 kV. As an application, the dc electric field distributions under various dc high voltages from 1 to 18 kV are measured with ac modulation parameters: 10 kHz and 0.5 kV. The dc electric field distribution, after being normalized by the mean dc field across the gap, is shown in Figure 6.16. 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Norwich, Information, Sensation, and Perception, (Academic Press, San Diego, 1993). [6-29] U. Gäfvert, A. Jaksts, C. Törnkvist, and L. Walfridsson, “Electrical Field Distribution in 161 Transformer Oil”, IEEE Trans. Electr. Insul. 27, 647 (1992). [6-30] B. Malraison and P. Atten, “Chaotic behavior of instability due to unipolar ion injection in a dielectric liquid”, Phys. Rev. Lett. 49, 723 (1982). [6-31] X. Zhang, J. K. Nowocin, and M. Zahn, “Effects of AC Modulation Frequency and Amplitude on Kerr Electro-Optic Field Mapping Measurements in Transformer Oil”, in Annual Report of CEIDP, Montreal, Canada, pp. 700-704 (2012). [6-32] M. Zahn, Y. Ohki, D. B. Fenneman, R. J. Gripshover, and V. H. Gehman, “Dielectric Properties of Water and Water/Ethylene Glycol Mixtures for Use in Pulsed Power System Design”, Proc. IEEE 74, 1182 (1986). [6-33] A. Törne and U. Gäfvert, “Measurement of the Electric Field in Transformer Oil Using Kerr Technique with Optical and Electrical Modulation,” in Proceedings, ICPADM, Vol. 1, Xi’an China, 24-29 June 1985, pp. 61-64. [6-34] T. Maeno and T. Takada, “Electric Field Measurement in Liquid Dielectrics Using a Combination of ac Voltage Modulation and a Small Retardation Angle,” IEEE Trans. Electr. Insul. 22, 503 (1987). 162 7 Concluding remarks In this thesis, it has been demonstrated both quantitatively and qualitatively that Kerr electro-optic measurements with a high-sensitivity CCD camera can be used for electric field mapping. Measurement accuracy and reliability for uniform and fringing space-charge free fields and field with space charge have been evaluated in Chapter 2. Generally speaking, the relative errors will be reduced as the applied voltage increases. This may not be true when the voltage approaches the breakdown threshold, since more uncertainties would be introduced due to high-field conduction and pre-breakdown phenomena in the liquid dielectrics. To further improve the sensitivity of the measurements, it is necessary to identify and quantify various sources of noise in the experimental system, including optical, electro-optical, and electrochemical processes. Image processing techniques may also be helpful to enhance the data quality. The most straightforward application of image processing algorithms in our measurements is edge detection, i.e. identification of the electrode surfaces in the images taken by the CCD camera. This would be more demanding when the oil gap is smaller, since the same edge detection inaccuracy (e.g. 5 pixels) takes up a larger portion of the gap. The smart use of charge injection to improve breakdown strength in transformer oil is demonstrated in Chapter 3. Hypothetically, bipolar homo-charge injection with reduced electric field at both electrodes may allow higher voltage operation without insulation failure, since electrical breakdown usually initiates at the electrode-dielectric interfaces. To find 163 experimental evidence, the applicability and limitation of the hypothesis is first analyzed. Although further efforts should be made to test more electrode materials, the present work clarifies a crucial issue regarding the hypothesis. To test the hypothesis, many experimental details need to be carefully considered, such as appropriate impulse waveform, similar intrinsic breakdown voltage of different electrode materials, and dynamic Kerr measurement before the onset of flow. Only under these specific circumstances, the hypothesis is testable and correct. Impulse breakdown tests and Kerr electro-optic field mapping measurements are then conducted with different combinations of parallel-plate aluminum and brass electrodes stressed by millisecond duration impulse. It is found that the breakdown voltage of brass anode and aluminum cathode is ~50% higher than that of aluminum anode and brass cathode. This can be explained by charge injection patterns from Kerr measurements under a lower voltage, where aluminum and brass electrodes inject negative and positive charges, respectively. More importantly, we worked out a feasible approach to investigating the effect of electrode material on the breakdown strength, which may be difficult and inconclusive to be directly related to the electronic, mechanical and thermodynamic characteristics of the metal. The complexity has been reduced to charge injection patterns and intrinsic breakdown strength. In Chapter 4, the fractal-like charge injection kinetics in HV pulsed transformer oil has been identified from Kerr electro-optic measurement data and verified by numerical simulations of the time-dependent drift-diffusion model with the experimentally-determined injection current boundary conditions. It is shown that while the space charge process in the liquid bulk is drift-dominated, the charge injection kinetics from the electrical double layer on the electrode-dielectric interface is diffusion-limited. Two mechanisms are proposed to reveal the deep connection between geometrical 164 characteristics of electrode surfaces and fractal-like kinetics of charge injection. The order of injection current densities is 10-5~10-3 mA/mm2 in our experiment, corresponding to total current of about 10-2~1 mA in the gap and bulk conductivity enhanced by 104~106. With such a large magnitude, it seems that the transient charge injection should be associated with the charging dynamics of EDL. Otherwise, the formative steps in Figure 4.2 would be the same as in previous studies which work only under long-term high-voltage applications, while the difference between transient (~1 ms) and steady-state (> 1 min) charge injection patterns in dielectric liquids has been found as early as in 1960s. A comprehensive consideration of the chemical aspects of the processes (chemical compositions, reaction schemes, etc.) is out of scope of this work and may be proposed for further studies. Chapter 5 explores the possibility of early warning of electrical breakdown initiation in high voltage pulsed transformer oil from the data of Kerr electro-optic measurements. Due to electrostriction, the detected light intensities near the rough surfaces of electrodes both fluctuate in repeated measurements and vary from pixel to pixel in a single measurement. The calculated coefficient of variation has a strong nonlinear dependence on the applied voltage, implying that some critical transitions are taking place, at least at some spots on the electrodes. The results of this work may be helpful to develop new approaches to non-destructive breakdown test and, based on the same physical principle, non-destructive inclusion detection in dielectric liquids. Additional work needs to be done to find more evidence that electrostriction is the major force behind the early warning signal. The influence of a strong electric field on a liquid is noticeable when the electric field energy density is comparable with the external pressure. This condition is usually satisfied in the case of breakdown initiation. We can place the test cell 165 inside a pressure chamber with a wide range of adjustable pressure. Theoretically, it is expected that the critical threshold of the applied voltage would be higher under higher pressures. Under the same applied voltage, the detected fluctuation in electro-optic signal should strongly depend on the ambient pressure. The influences of applied voltage (peak, rise time, polarity), electrode material and surface roughness, and ambient pressure on the electrostriction effects need also be investigated. In the field of dielectric and electrical insulation research, the most common impulses are microsecond instead of nanosecond. We will start from nanosecond rise-time pulses and gradually increase the rise-time to the microsecond range. By doing this it is possible to find a characteristic time beyond which the space charge behavior dominates. Since parallel-plate electrodes are used, we do not expect any polarity effect if the two electrodes are ‘identical’. This can be a basic check of the reliability of the measurement results and the processed data. We would also like to propose experimental procedure on the non-destructive inclusion detection. Prepare transformer oil with conductive inclusions of nm to µm diameter range. The first type is a dilute nano-fluid; the second type is to release a small number of conducting micrometer-size suspensions between the two electrodes. Test transformer oil samples with these controlled conducting inclusions to measure the resulting local electric field enhancement which can be a trigger for electrical breakdown or partial discharge. This method can easily be extended to larger scale industrial systems by scanning the entire liquid region. In Chapter 6, experimental studies are carried out to find temporal, spatial, spectral, and correlational electro-optic signatures of turbulent electroconvection in transformer oil stressed by dc and ac HV. The implications of this work are two-folded. Combining theoretical models 166 of optical wave propagation in turbulent medium and statistical characteristics of simulated electroconvective turbulence fields, it might be possible to test and verify numerical results with experimental data. Moreover, this work also clarified some important issues on Kerr electro-optic measurements. The results presented in Section 6.2 refreshed the understanding of the term “steady state” in dielectric liquids stressed by HV, which is meaningful only in statistically averaging sense. The last section demonstrated that to reduce the influence of flow on the optical detection of harmonic components, the modulation frequency should be high enough; and the lower ac amplitude is also desirable. * * * This thesis is an interdisciplinary research involving, in general terms, material science, electrical engineering, computer science, mechanics and physics. It makes contributions to the areas of electrostatics, electro-optics, electrochemistry, and electrohydrodynamics. However, the story is far from finished yet. The goal of constructing an integrated picture of physical processes in high-field stressed dielectric liquids has not accomplished. On this subject, future work can be done in three directions: (a) A detailed analysis of the chemical composition in transformer oil and reaction schemes involved in electrical conduction; (b) A numerical model incorporating the dynamics of electrical, chemical, mechanical and thermal processes with the simulation of electrical birefringence and optical propagation; (c) An integration and optimization of the optical system based on careful investigation of the optical property of each component. The proposed work will advance the knowledge on a more fundamental level. From an even broader perspective, my thesis provides foundations for a long-term research on advanced 167 materials in power engineering and energy technology. For example, the same measurements can be done with dilute transformer oil-based nano-fluids, the importance of which has been recognized by ABB researchers. The behaviors of thin films and colloids in electric field have received considerable research interests in recent years. Porosity of dielectrics and electrode coatings, and nano-patterned electrode surfaces may result in unique mechanical and electrical properties. The use of an ultrafast laser may enable us to explore some more complex electrooptic phenomena. Some semiconductors and inorganic materials may be utilized to make super-capacitors. 168 Bo Suan Zi: Ode to Plum Blossom by Lu You (1125−1210), great poet of China’s Song Dynasty (Translation adapted from Dict.cn) By a broken bridge outside the post-hall, Blooming lonely, no care does she gain. Though drowned in sorrows at night-fall, She still suffers much from wind and rain. For the first of spring she has no lust, Just let spring flowers envy her fame. Even fallen in mud and ground to dust, Her fragrance still remains the same. 169 170 A Physical and chemical parameters of transformer oil Shell’s Diala® A oil meets the ANSI/ASTM D3478 and the NEMA TR-P8-1975 specifications. It is formulated with refined petroleum oil and a lubricant additive. Their inherent toxicity is quite low. However, prolonged or repeated contact requires the observation of good industrial hygiene practices. Table A.1. Physical and chemical parameters of transformer oil Properties ASTM test method Typical Values Interfacial tension, 25 °C, dynes/cm D971 45 Specific gravity, 15/15 °C D1298 0.886 Viscosity, cSt at 40 °C D445 9.37 Viscosity, cSt at 0 °C D445 66 Dielectric breakdown voltage at 60 Hz, kV D1816 28 (VDE electrodes, 1.02 mm gap) Dielectric breakdown voltage impulse, kV D3300 176 (25.4 mm gap, needle-to-sphere GND) Oxidation inhibitor content, %w D2668 None Sulfur, %w D2622 0.07 Water, ppm D1533 30 Oxidation stability (164 hrs, sludge %w) D2440 0.15 Gassing tendency, l/min D2300 16 Coefficient of expansion, ml/°C /ml D1903 0.00075 171 Table A.1 (continued). Physical and chemical parameters of transformer oil Properties ASTM test method Typical Values Dielectric constant at 25 °C D924 2.2 Thermal conductivity, cal/cm/sec/°C D2717 0.0003 Molecular weight D2503 261 Refractive index D1218 1.4815 Viscosity-gravity constant D2140 0.865 Carbon type composition: %CA D2140 7 Carbon type composition: %CN D2140 47 Carbon type composition: %CP D2140 46 172 B Approaches to improving breakdown strength in liquids 1 Introduction In the first part of this Appendix, a brief overview of electrical breakdown in liquid dielectrics is presented, which serves as preliminary knowledge for the subsequent parts. For more details, one can refer to some textbooks on high voltage engineering [1~4]. Efforts to understand breakdown mechanisms in a variety of liquid insulants have been continuing for many decades. However, unlike gases and solids, there is no single theory that has been unanimously accepted. This is because the molecular structure of liquids is not simple and not so regular. For instance, transformer oil, the most common dielectric liquid, contains well over 100 chemical compounds, and the fact that liquids tend to be contaminated with various impurities is a serious problem for fundamental studies. Moreover, the transition from liquid to gas phase, which takes place during the development of breakdown, still further complicates the phenomena and hence their interpretations. From the experimental studies of breakdown process, the breakdown of liquid is influenced by various factors such as experimental procedure, electrode geometry, material and surface state, presence of chemical and physical impurities, molecular structure of liquids, temperature and pressure. Several breakdown theories like electronic theory, suspended particle theory and bubble theory were advanced in the late 1960s, resulting in. However, it is clear that no single concept in these 173 theories can explain all experimental observations in a unified manner, and it has been necessary to modify and sometimes even reject them with the emergence of new experimental evidence. For instance, the electronic breakdown theory which was an extension of electron avalanche concept in gas discharges has been rejected due to no direct experimental evidence for the avalanche process. Thus, in the following sections, we will only introduce other more promising hypotheses based on particle and bubble effects and observation using optical techniques. With the advent of fast electro-optic techniques, the understanding of breakdown in liquids has been advanced tremendously. With these techniques, once a voltage pulse is applied any perturbations occurring in the electrode gap can be easily visualized under magnification by taking a photograph of each event. Verification of the bubble theory was conducted using ultra high speed photography, which confirmed that streamers emerge from the high voltage electrode grow out in the liquid toward the opposite electrode if the field is critical, and that actual breakdown is preceded by the formation of secondary streamers which grow faster than the primary ones. The most popular methods that have been used are shadowgraph/schlieren techniques, Kerr electro-optic techniques and holographic techniques. However, the characterization of breakdown process is out of the scope of this research. 2 Suspended particle breakdown theory Suspended particles are always an integral part of liquids. In spite of rigorous cleaning techniques imparted both on liquids as well as test cells, submicron sized particles cannot be removed from the system. The particles could be a fiber, probably soaked with moisture, or it may be even a droplet of water. The relative permittivity of these particles is higher than that of 174 the liquid. Assuming them to be spherical, then the particles will experience a force that is directed toward areas of maximum stress. Therefore the particles will align on the high stressed electrode and start forming a bridge which could lead to gap breakdown. Similarly if particulate matter is fiber it will get polarized due to the presence of moisture on its surface and move along converging fields. When a fiber reaches either electrode, its outward tip would act as extension of the electrode, cause field intensification and thus attract more fibers, thereby forming a bridge in the gap. This can lead to breakdown via joule heating of the bridge and its surrounding liquid. The evidence in support of this theory includes the increased time required to reach dc and ac breakdown of the liquid with increased viscosity, while under high-frequency or fast impulse voltages this phenomenon does not occur. Although this theory did explain the breakdown in liquids containing large amount of particles, it is unlikely to be extended to pure liquids. Moreover, particles have been seen on several instances to bridge the gap, while discharge occurs in a different region and still at higher voltages. This means breakdown involves some other mechanisms. Nevertheless, particles may be instrumental as an aid in the process of breakdown. 3 Bubble theory of breakdown According to this theory, a low density vapor is generated in the liquid by the injection of large leakage currents at the electrode protrusions. By this process local vaporization can occur in a few milliseconds. Calculation of the heat needed to vaporize a liquid is straightforward in heat theory. Near breakdown the emission current from the cathode is space charge limited and is given as proportional to an exponential form of the local field. It then 175 follows that the local energy input during the applied high voltage pulse duration can be expressed as a function of the local electrical field. The critical breakdown field strength can be solved by equating the energy input and the energy required to vaporize the liquid. This is the so-called thermal breakdown criterion and exhibits a marked pressure and temperature dependence since the boiling temperature increases with pressure. If the liquid is degassed, its breakdown strength becomes less dependent on the pressure. This theory also explains the effect of molecular structure of the liquids on breakdown. However, the main objection to this model has been the simple heat transfer treatment based on the steady state equation for a phenomenon which indeed needs to be described by transient heat flow dynamics. In this theory, the concentrated field at electrode protrusions would play a basic role. Three other alternatives have been proposed to account for the formation of gas bubbles: release of occluded gases from micro-pores in electrode surface layers; cavitations caused by mechanical strain of the liquid under the highly concentrated electric field with corresponding electrostrictive pressure differential; and electrochemical dissociation of some liquid molecules with the release of gases. 4 Factors influencing breakdown strength of liquid dielectrics A) Temperature and pressure The effect of temperature on electrical strength of an insulating liquid depends on its type and degree of purity. For example, the breakdown strength of dry transformer oil is insensitive to temperature except slightly below the boiling point, where the breakdown strength decreases drastically probably because of the formation of vapor bubbles and their growth aided by the decrease at such temperatures of the oil’s viscosity and surface tension. The breakdown strength of oils that have a trace of moisture are sensitive to temperature 176 variations over the full range from about -20°C up to their boiling point of about 250°C. The breakdown strength of an insulating liquid under dc and power frequency increases significantly with applied static pressure. Raising the pressure from atmospheric to 10 times higher increases the breakdown strength by about 50%, depending on the type of liquid. Another effect of pressure is the suppression of pre-breakdown discharges. These observations support the bubble theory of liquid breakdown. However, under very fast impulse voltages of duration less than 0.05 μs, breakdown voltage is insensitive to both pressure and temperature. B) Electrode and gap conditions The breakdown voltage of a liquid insulated gap depends on its width as well as the electrode shape and material. For gaps with highly non-uniform fields such as that of a pointto-sphere gap, there is a polarity effect. The negative DC breakdown voltage is lower than the positive voltage up to a critical gap length above which the relation reverses. This critical gap length depends on the liquid and the electrode material. There seems to be no simple explanation for these phenomena. However, the material of the cathode surface layer determines the electric stress necessary for electron emission. These electrons play a decisive role in the conduction and breakdown processes. The size and shape of electrodes determine the volume of liquid subjected to high electric stress and the degree of field nonuniformity. The bigger this volume is, the higher the probability of its containing impurity particles. The more of these particles that are present, the lower would be the breakdown voltage of the liquid gap. Moisture is also an important factor. The sensitivity of liquid breakdown to these factors is logically higher under DC and powerfrequency AC than fast impulse voltages. Thus the impulse ratios of highly non-uniform gaps of contaminated or technically pure liquids can reach about 7. 177 It has also been shown that, stressing the oil gap under high-voltage for a long time, and repeated sparks of limited energy, tend to raise the breakdown voltage of the gap. This is called conditioning. Particles in suspension collect at zones of field concentration. Points of microroughness on the electrodes get eroded by concentrated discharge currents. A film of discharge byproducts gradually covers the discharge areas of both electrodes. In the case of the silicon oil, repeated breakdowns tend to cover the electrodes with a film gel and solid decomposition products. If a high-frequency arc is allowed to take place in the liquid gap, the arc products cause the liquid properties to deteriorate. C) Impurities Impurities include solid particles of carbon and wax, byproducts of aging and discharges, cellulose fibers, residual of filtration processes, water, acids, and gases. Impurities usually cause a reduction in the electrical breakdown strength of an insulating liquid, the largest effect being that of the simultaneous presence of moisture and fibers. Cellulose fibers are known to be hygroscopic. Thus, floating moist fibers tend to bridge the oil gap. Under both DC and AC the effect of a trace of moisture is drastic on meticulously dried liquids, much greater than that of commercial liquids. The effect of moisture is less pronounced in the case of oil gaps with strongly nonuniform fields and with liquids containing no fibers. Because water solubility is considerably higher in silicon oil and phosphate esters than in mineral oil, they need to be much more carefully dried and kept. Metal particles may be present in dielectric liquids, particularly those used in transformers and circuit breakers. Their presence reduces the breakdown strength of oil by as much as 70%. Longer and thinner particles contribute more to the reduction of the oil’s breakdown voltage. 178 D) Flow The behavior of transformer oil and other dielectric fluids used for the cooling and insulation of power system equipment is significantly influenced by the motion enforced by the action of circulating pumps. Two important factors affect the situation. First, charges generated by streaming electrification in critical parts of the hydraulic circuit having high velocity and/or turbulence can accumulate to distort the electric field in positions where dielectric integrity is prejudiced. Also, the dielectric strength of the fluid is altered by the actions of the flow. Charge separation at interfaces between a moving fluid and a solid boundary can give rise to the generation of substantial electric fields. Either alone or in combination with the existing electric fields imposed by the energization of the equipment, these can give rise to insulation failure. The initial response of apparatus manufacturers has been to reduce design velocities and curtail the operation of pumps. In apparent contrast, during standard oil testing, the continuous flow of oil was found to increase the mean breakdown strength. The increase depends on the electrode material and is larger with steel electrodes than with brass. The increase of breakdown strength can be explained by assuming either that the oil flow impedes the entry of impurities into the gap, or that the oil motion delays the establishment of particle bridges between the electrodes. The change in breakdown strength was significant with an oil velocity of 3 cm/s, although a much higher velocity is needed to have such an effect. To further complicate the picture, excessive increase in oil velocity causes the flow to become turbulent, where gas bubbles may then be created which lead to a reduction in breakdown strength. 5 Review of Ref. [5] The author had realized that Townsend-type theory was not successful in liquid 179 breakdown. Also in the author’s opinion, the conductivity of liquid insulators is mainly due to ions while breakdown should be ascribed to coarser particles. The author applied the electrostatic theory to colloid chemistry, and the insight into the mechanism of breakdown became much clearer. The key point of this book can be stated as: the electric strength of liquid insulating material depended mainly on its degree of purity. According to the author, contamination of insulating oil is unavoidable owing to various factors. The simplest physics picture is: colloid particles of high permittivity will be charged in oil, i.e., absorb an amount of positive ions and collect an atmosphere of negative counter ions and dipoles or absorb soaps. They may tend to unite by flocculation as a result of which the particles after a collision may adhere, whereas their ion atmospheres unite and form a single atmosphere enveloping the enlarged complex. This flocculation depends on the relative magnitudes of the attractive London-van der Waals and chemical binding forces between the particles and the repulsive electrostatic forces between the ion atmospheres. The repulsive interaction energy increases in proportion to the particle size, while the breakdown strength goes downhill. Therefore an equilibrium state with maximum particle size and lowest electric strength will be reached. Both theory and experiment indicate that for the formation of a bridge only particles of high permittivity and larger colloid sizes are responsible. When the particles increase in size the breakdown strength goes downhill. The non-uniformity (global or at least local) and impurities of high permittivity are two factors effectuating breakdown. The non-uniformity of the field in the gap is due to its finite dimension (the unavoidable existence of edges) and the non-smoothness of the electrode surface (the protrusions or attached contaminants induce local stress concentration to at least 2- 180 3 times the average value). When impurity particles in non-uniform field have a high permittivity, they will be polarized with a gradient force proportional to the square of local field imposed. So they will drift towards a place of maximum stress where they align head-totail to minimize the free energy. If the stress exceeds a certain limit, a bridge will be formed as a consequence of flocculation which is necessary to cement together the elements of the bridge. Electrical discharges were observed between parts of a bridge which had been disrupted by gas bubbles developed by Joule heat or electrolysis. Pre-breakdown discharges may occur which do not develop into a real destructive breakdown with unlimited carbonization but may result in development of gas in colloid suspensions. Corona discharges in gas bubbles and local heating in bridges may cause the amount of carbon particles and the acidity and soap contents to increase, which lead to deterioration of the dielectrics. Meanwhile, however, the liquid may be purified by electro-deposition of the impurities at dielectric interfaces or electrodes. In a breakdown or a pre-breakdown discharge controlled by a large series resistance, no important additional carbonization and formation of acid in the oil occurs and the impurities may have disintegrated. This conditioning effect is the opposite of flocculation. In this case a second breakdown may happen at a stress higher than the first breakdown. A certain conditioning effect may also take place by electrostatic precipitation of the impurities at a third electrode. This electro-deposition may be obtained by relatively low field intensities. To improve the breakdown strength, in addition to efforts to keep the electric field in the insulation as uniform as possible, the principal advice to be gained from this book is: to see it that the insulation is pure. A short survey was given of different methods of purifying the insulating oil, including methods of washing with fuming or concentrated sulphuric acid and distillation. Good results and extreme purification of hydrocarbon oils were obtained by 181 removal of tiny particles in a Cottrell filter. However, this method failed for oils with a permittivity close to that of the impurities. Moreover, in this case, centrifugation proved also to be disappointing. Addition of a suitable soluble compound to an insulating liquid may increase the breakdown strength or prolong the life by preventing flocculation. The compounds used should be added in a definite, minute concentration. A colloid chemical stabilizer (such as anthraquinone which is a chemically stable, heavy aromatic compound) can prevent the flocculation, whereas the so-called scavengers (such as tin tetraphenyl) may be applied to remove deterioration products. The removal effect of natural inhibitors may increase the breakdown strength, but the rate if deterioration of the mineral oil may thereby accelerated. The action of several inhibitors appear to consist of tightly binding acids, oil molecule radicals and iron sludge particles and forming insoluble compounds, or providing impurities with an aromatic cover to prevent further flocculation. The breakdown strength depends on the duration of the application of the field, the waveform of the applied field vs. time and in general on the past history of the insulation. In liquid dielectrics, with time-lags of a few microseconds (the time it takes for particles to join into a bridge), the breakdown strength may be shown to decrease dramatically with the increase of the duration of application. After about 1 millisecond a more constant value of breakdown strength is reached. In a well-controlled breakdown or a pre-breakdown discharge, if no additional carbonization of the oil has taken place, the complexes consisting of impurities may have disintegrated, which follows that the diameter of particles decreases whereas their number 182 grows. The author derived relations between breakdown strength EB and characteristic size of particles r as follows: for long-time cases, EB r3/2 =const; for short-time cases, EB r7/4N1/2 =const where N is the total number of particles. Owing to the disintegration effect, the original shorttime breakdown strength has decreased (from some intrinsic breakdown strength which is ionic in origin instead of electronic), while the long-time value has increased. A phenomenon often reported in the measurements of the breakdown strength is the influence of the gap width between electrodes. In general the strength decreases with the increase of the gap width, but after the gap distance has reached a magnitude of a few millimeters it will remain constant. The effects of space charge were also discussed. The space charge may be ascribed to ions as well as to colloid particles and permanent dipoles. Space charge may cause the dc breakdown strength to increase if the space charges are rigidified at the interfaces, which strongly retard the flow of the colloid particles toward a place of maximum stress. 6 Review of [6] In spite of the title of the book, the discussions of liquid breakdown only appear in the last two chapters. The first 18 chapters were devoted to an excellent establishment and demonstration of ionization and conduction phenomena in electrically stressed liquid. The author aimed at explaining various experimental facts from fundamental principles, i.e. combining the microscopic molecular structure and electronic orbit properties and the hydrodynamic descriptions and the chemical kinetics on macroscopic level. This is quite successful. So no wonder the author showed his preference on electronic breakdown theory as a natural extension of his theory on ionization and high-field conduction. Although this theory 183 for breakdown has been rejected, there remains much valuable information in this classic book. In Chapter 19, the author did not introduce his theoretical ideas. Instead, he reviewed a lot of previous experimental investigations. The influence of electrode materials, impurities and additives in the liquid, gas content, degassing of the liquids and electrodes, the duration of the voltage applied, the rate of increase of the applied voltage and the frequency of ac voltages, and the effect of temperature and hydrostatic pressure are included in this chapter. In Chapter 20, the author, according to the known experimental results, developed his theory and compared it with many other existent theories, which will be commented in a later section. If not explicitly stated, it is impulse breakdown that serves as the main approach to investigate the liquid breakdown strength. As shown in Figure B.1, there exists a minimum pulse duration τ0 for which a constant value of the impulse breakdown is obtained. For very short pulses with duration smaller than τ0, the electrical strength goes downhill with the increase of pulse duration. Figure B.1 (from Ref. [6]). Dependence of breakdown strength Ebd (MV/cm) on time τ (μs) in saturated hydrocarbons with gap separation of 63.5 μm: a, hexane; b. heptane; c, octane; d, nonane. Besides the dependence on pulse duration, the great amount of experimental work has pointed out several other quantitative relationships. The most important are: Breakdown field stress increase proportionally with increase in the density of the liquid, as shown in Figure B.2. 184 Figure B.2 (from Ref. [6]). Dependence of breakdown strength Ebd (MV/cm) on liquid density ρ (g/cm3) under various experimental conditions: a, normal paraffin, τ = 1.4 μs; b, single branched-chain hydrovarbons, τ = 1.4 μs; c, double branched-chain hydrocarbons, τ = 1.4 μs; d, normal paraffin, direct voltage; e, single branched-chain hydrocarbon, direct voltage; f&g, straight and branched-chain benzene derivatives, τ = 1.65 μs; h, silicons, dc. The electrical strength of chemical substances with a molecular structure including branched chains (isomers) is lower than those with a straight chain molecular structure. Breakdown strength for liquids belonging to the aromatic hydrocarbons is in general greater than that of saturated hydrocarbons. The effects of electrode material have also been shown. In Figure B.3, the relation between breakdown field and electrode spacing is shown for different electrode (in point-plane configuration) materials (Al, Cu, Cr) in hexane. When the point electrode is negative, there is no difference for the three materials, but when the point electrode is positive the breakdown stress increases from Al to Cu to Cr. Figure B.3 (from Ref. [6]). Dependence of breakdown voltage Vbd (kV) on electrode separation δ (μm) for a number of electrode materials and cathode shapes: flat cathode: a, Cr; b, Cu; c, Al (flat cathode); d, Cr, Cu, Al (point cathode). 185 Very interesting results have been obtained during studies of the relation between the breakdown strength and the number of breakdowns under dc conditions. As indicated by Figure B.4, this conditioning effect may cause the breakdown strength to increase by about 50% -100%. After a large number of breakdowns, due to the contamination of the liquid, there may be a drop in breakdown stress. Figure B.4 (from Ref. [6]). Dependence of breakdown strength Ebd (kV/cm) on the number of breakdowns N in transformer oil. The dashed lines indicate the limits of scatter of experimental results. An increase in the temperature of the liquid usually causes a reduction in the electrical strength, which can be explained by the reduction of the density and viscosity. The relation between breakdown stress and temperature for paraffin and silicon oils is shown in Fig. 5. The dramatic drop near the boiling point of the liquid can also be observed. The dependence of breakdown field on hydrostatic pressure relies on the amount of air dissolved in the liquid and absorbed by the electrodes, and also on the duration and polarity of applied pulse. For pure liquids, the breakdown strength increases with pressure. This book only provides experiments under low pressure (< 1 atm). However, later experiments indicated that at pressure of 25 atm breakdown strength will further increase, whereas the mean free path of the electron, according to electronic breakdown theory, is hardly altered. 186 At very high fields and with such a great dose of radiation (in megarads) that the effect of ionizing radiation is comparable with that of the electron emission, a significant irradiation effects has been observed. For example, irradiation caused an increase in breakdown stress of about 100%-300% for polyethylene at temperatures above melting point. Adding different substances to the liquid may lead to a decrease (e.g. water) or increase in breakdown strength. For instance, it has been reported that the addition of iodine to oil in an amount of 0.01 g/litre increased the breakdown stress by 18%, but a greater amount (about 0.1 g/litre) reduced the breakdown stress by 5%. Great attention has been paid to the possibilities of increasing the breakdown strength by adding suitable additives. It was found that the proper addition of p-nitrotoluene to cable oil may increase its electric strength by 48%. The more volatile additives proved to be more effective than non-volatile ones in liquid paraffin tests. The effect of selenium was very pronounced and was attributed to the possibility of the formation of a protective layer on the electrode surfaces. Two distinct optimum values were found, the lower one for maximum reduction of conduction current and the higher one (one order higher) for maximum increase in breakdown stress. The presence of electronegative oxygen in the liquid may also produce a double layer next to the electrodes which reduces the emission from the cathode. It has been shown that in hexane the influence of oxygen causes the electric strength to rise from 0.7 MV/cm to 1.3 MV/cm. Studies of the effect of frequency on breakdown strength in dielectric liquids are of great importance in radiotechnology. For low frequencies (dc–power freq. ac) the breakdown strength for hexane and oil increased with frequency by about 60% to 70%. For high frequencies (> 1 MHz), the breakdown strength fell toward zero with increased frequency. It 187 was supposed that thermal breakdown took place at very high frequencies. On the other hand, the effect of impurities and additives is more pronounced at low frequencies than at high frequencies. For oil, it was found that filtration and removal of water increased the breakdown strength by about 3 times at 50 Hz but only by 1.3 times at frequencies of the order of 100 kHz. In general it could be said that some theories explain the breakdown mechanism using a macroscopic interpretation such as heat production in certain places in the liquid especially at the cathode, the presence of impurities, colloidal suspensions, gas bubbles and vapor bubbles, non-uniform distribution of the electric field, irregularities on the cathode surface, etc. Other theories consider the mechanism from a microscopic view and derive the breakdown criterion on the basis of molecular structure. The first group refers to experimental conditions in which liquids of a commercial grade are used, which are not properly cleaned and degassed, and when relatively large conduction currents and long duration of the fields are applied. Such conditions are used in most of the industrial and commercial work, and for this reason these theories are acknowledged and find application. Theories connecting the phenomenon of breakdown with molecular structure of the liquid refer to experimental conditions where it is possible to observe the physical mechanisms of the phenomenon regardless of the purity of the liquid. In the author’s opinion, they form a basis for establishing a breakdown criterion and their study could lead to very important future applications. At the end of this book, the author compared various theoretical hypothesizes with experimental results, which we think is the most valuable part of this book providing a good basis for future theoretical development of liquid breakdown. 188 7 Review of [7] This monograph is the first attempt at a comprehensive consideration of electrical insulation in high-voltage electro-physical systems. The operating conditions of high-voltage system insulation and the requirements imposed on it are analyzed and the main insulation design types are outlined in the first part of this book. In the second part, information on shortand long-term electric strengths of vacuum, gas, liquid, solid and hybrid dielectrics as functions of various influencing factors is presented. Close attention is also paid to an analysis of various ways to improve the insulating characteristics of dielectrics. The remaining part of this book is devoted to the design of high-voltage insulation systems. Methods of increasing working field strengths and calculating the static, volt-second and statistical characteristics of the electric strength of insulation and the insulation service lifetime and reliability are considered here. This is the English version of a Russian book, most of the references of which were published in Russian. So, we think what this book tells is actually the results from the Russian (or more exactly, the former Soviet Union) investigators. Factors influencing the electric strength, according to the author, include dielectric material properties and states (pressure, density, viscosity, temperature, molecular and supermolecular structures, mechanical stress condition, etc.), electrode material and state of the electrode surface, contaminations (solid particles, moisture, and gases dissolved in the liquid and adsorbed on the electrode), polarity (for dc and impulse), type (for ac, frequency is also a factor) and duration (for pulses) of the voltage, insulation gap geometry and other environmental conditions. All the material covered is of great interest to experts in research areas and industries of power systems and electrical insulation. 189 We only focus on the contents that indicate comparisons of liquid breakdown strengths under different conditions, or can be directly related to the improvement of electric strength of liquid insulations. These contents are summarized in Table B.1. Table B.1. Dependence of electrical breakdown strength of insulating liquids on various factors (extracted from Ref. [7]). Factor Dependence Implication or Example Pressure a. After careful liquid degassing the influence of pressure on electric strength sharply decreases, according to the bubble theory; polar and conducting liquids are exceptions because liquid gases are rapidly produced as a result of currents and dielectric losses. b. The effect is much stronger for a homogenous field than for inhomogeneous field. In the former case gas accumulated at electrodes and subjected to pressure has a major effect on breakdown initiation. c. For long-term applied voltage, the probability of gas formation increases. Thus the dependence is also strengthened. a. For very pure liquids under short-term voltage exposure, the main effect of temperature on electric strength is due to the temperature-dependent density. The electric strength slowly decreases with the increasing temperature. And the decrease in voltage duration weakens this effect. b. For commercially pure liquids containing impurities and under long-term voltage exposure, the temperature dependence is mainly due to the temperature-sensitive moisture and gas contents. In addition, the viscosity, surface tension and the hydrodynamic flows must be taken into account. So the dependence may be rather complex. It is often desirable to raise the hydrostatic pressure to increase the electric strength of liquids in the following cases: 1) for liquids with high electrical conductivity (water, glycerin, alcohol, etc.); 2) for large electrode areas (with more homogeneous field); 3) for long voltage pulses (>1 μs). a. The dependence of electric strength on electrode material is perhaps due to the variations in the work function for electrons going from metals to liquids, the Young’s modulus and thermodynamic characteristics. b. There was evidence that, the electric strength of liquid was mainly affected by the anode material. The reduction in electric strength of cryogenic liquids with decreased Young’s modulus of electrodes was also revealed. Electric strength of purified water and hexane for hemispherical electrodes (0.2 cm in diameter, and 200 μm in separation) made from indicated materials. Temperature Electrode Material 190 Dependence of electric strength of in-service (1) and dried (2) transformer oil in a standard breakdown system. Factor Dependence Implication or Example State of Electrode Surface a. The effect of electrode contamination and oxidation on the electric strength is two-fold. For short-term voltage applied, the oxide film increased the electric strength for short gaps. For long-term exposure, the reverse effect occurs. b. The reduced influence of electrode microgeometry due to a local increase in electrical conductivity of the medium can be used to increase the electric strength of gaps with liquid insulation Negative effect. Filtration is necessary for the improvement of electric strength. 1. Careful electrode degassing increases the electric strength of degassed liquids for dc and ac voltages by 15~20%. 2. Shielding the electrode surface by ionic layers and heating the volume of liquid adjacent to micro-tips by high-voltage conduction currents are two means to increase local electrical conductivity. Negative effect. Drying process is also essential to ensure the quality of liquid insulation. Dependence of Ebr on relative humidity for commercially pure oil (1) and oil with 0.005% of cellulose fibers (2). Gap Width Generally speaking, the longer the gap is, the lower the breakdown stress will be. However, certain exceptions have been reported. Dependence on center electrode radius of Ubr in transformer oil for an electrode system comprising coaxial cylinders with an outer-cylinder radius of 100 mm and ac voltage at 50 Hz. Electrode Surface Area Radiation This effect decreases with decreasing voltage duration. Large electrode reduces electric strength (lower-law relation) In some cases, the dependence of the electric strength of liquids on the dose or exposure time is displayed by a curve with a maximum. Solid Impurities Moisture The physical processes involved and therefore the dependence are extremely complicated. 191 Electric strength of transformer oil for 50-Hz ac voltage versus clearing method Factor Magnetic Field Dependence A transverse magnetic field hinders the multiplication of charge carriers and hence the onset of breakdown. Implication or Example Dependence of breakdown voltage of benzene (1 and 2) and toluene (3 and 4) on transverse magnetic field induction for interelectrode gap length of 1 (1), 1.15 (3), 1.7 (2) and 2 mm (4). Flow A liquid flow significantly influences electrical strength which decreases when discontinuities arise in the medium and the gas phase is formed in a turbulent flow, the number of weak regions in the inter-electrode gap carried by the liquid flow increases, and electrification of the liquid, changing of the insulator surface and the electric field distortion due to this changing dominate. On the other hand, however, the breakdown voltage increases when bubbles and gas phase nucleation centers predominantly escape from the strong field zone and from the hot liquid zone; bridges between the electrodes formed by solid and gas impurities and moisture drops are destroyed, and fragmentation of large gas bubbles and moisture drops into small-scale ones takes place. For pulses, the increase effect has been found for dried transformer oil filling in a coaxial cylinder electrode. Behavior of Ubr (50 Hz) for purified transformer oil exposed to voltage pulses (1), dc (2) and effective ac (3) voltages. Electrode Coating a. The positive effect of this method depends on many factors, including the coating parameters (thickness and material), the initial state of the electrode surface, the properties and state of the insulating medium (mainly its contamination), the electrode configuration and area, and the voltage type. The increase in breakdown voltage due to the use of thin dielectric coatings of the electrodes results from the joint or individual effect of several factors. b. In most cases, a positive effect is observed for DC and AC voltages. For impulse voltages, when the electric strength of dielectric liquids approaches that of solid dielectrics and impurity bridges are not formed, the effect is manifested only weakly. But there are publications in which the breakdown voltage in this case can be increased by 20%-25%. Generally speaking, it has been found that, both electrodes must be insulated to increase pulsed breakdown voltage. The positive effect of electrode insulation intensifies when aromatic additives (like anthracene) are injected into the oil. 192 8 Review of [8] Interest in the liquid breakdown under lightning pulses and in particular, internal surges has quickened in connection with an expansion of working voltages of electric power transmission lines and substations and the tendency to a decrease in the insulation level of high-power electrical equipment systems. The knowledge of the electric breakdown of liquids, however, has not kept pace with the increasing interest and more and more stringent requirements on liquid dielectric insulation design. This book is devoted to a description of physical mechanisms of initiation and propagation of pulsed discharges in liquids as well as to the basic laws describing impulse electric strength of liquids. It can is a specialization of another book of the author, which we just reviewed. As the author stated in the preface, in the process of writing, they had generalized the results of modern research and re-analyzed and reexamined a large volume of data on liquid dielectric breakdown obtained in the last decades. This has provided their deeper understanding and interpretation. In our opinion, this book can be regarded as a handbook for theoretically modeling the electrical breakdown phenomena in liquids. At the current stage, Chapter 6 of this book is what we concern most, which discussed basic laws describing of the impulse electric strength of liquids. In the subsequent sections, we will introduce the main results respectively. Duration, shape, frequency and polarity of voltage pulses In breakdown of liquids in a uniform field at times approximately by an order of magnitude greater than in gases, an increase in the electric strength is observed with decrease in the voltage pulse duration. In addition, a decrease in the duration of the applied voltage pulse decreases the role of gas formation in the discharge ignition and propagation. In short 193 gaps with a uniform field, this is manifested through changes in the discharge mechanisms for exposure times less than a certain critical one, namely, transition from the discharge from cathode (the bubble breakdown mechanism) to the discharge from anode (the ionization breakdown mechanisms or combined). In long gaps, changes in the voltage pulse duration (and, correspondingly, in the overvoltage magnitudes) are accompanied by changes in the external shape of the discharge figure and conditions of bush-like figure transformation into a treelike figure. For pulses with duration of several nanoseconds, the electric strength of even commercially pure liquids exceeds 1 MV/cm; it reaches 4MV/cm in a uniform field for duration t ≈ 4 ns and gap length d=1.25 mm. Moreover, liquids with radically different composition have electric strengths close in values. Under exposure to voltage pulses of equal durations the electric strength of liquids differs for pulses of different shapes demonstrates that the pulse duration is the important but not unique parameter of the voltage pulse that determines the electric strength of liquids. This circumstance stimulated a search for voltage pulse parameters that influence the prebreakdown processes in the liquid and, as a result, its electric strength. It was established that in long air gaps, the character of discharge processes and the breakdown voltage essentially depend on the slope of the oblique voltage pulses. An increase in the slope (from 0.4 to 600 kV/μs) causes the discharge ignition voltage to increase. However, for extremely small end radii of tip electrodes, the discharge ignition voltage increases as the pulse slope decreases. As shown in Figure B.5, for pulse duration of several tens or hundreds of microseconds, the dependences of the breakdown voltages in insulating liquids on the pulse slope have complex character. 194 Figure B.5 (from Ref. [8]). Voltage-time characteristics of a transformer oil with tip-plane gap configuration for d = 5 (1), 15 (2), and 25 cm (3). Under the joint influence of different voltage types applied in succession, the earlier voltage significantly affects the electric strength in the presence of the later. The electric strength increases if the polarity of previously applied voltage (pre-stressing) coincides with that of the applied voltage (for which the electric strength is measured). The maximum effect reaches tens of percent and depends primarily on the duration and magnitude of previously applied voltage, the time interval between the previously applied and applied voltages, and the type of voltage for which the electric strength is measured. The electric strength of liquid dielectrics at low frequencies (up to several kilohertz) depends weakly on the frequency. When dielectric losses in a liquid are insufficient to heat the liquid to temperatures of electrothermal breakdown, the electric strength of the liquid in a uniform field is independent of the frequency or slightly increases with the frequency. The latter is typically recorded for moderately pure liquids. The electric strength of commercially pure insulating liquids for the voltage at the industrial frequency is slightly (10–20%) higher than for dc voltages. The frequency dependence under a sharply non-uniform field with intense cavity processes, typically observed at relatively low ac electric fields, is U-shaped at frequencies of several hundred Hz, as shown in Figure B.6. 195 Figure B.6 (from Ref. [8]). Dependence of breakdown voltage of perfluorohaxane on the frequency in the tip-plane gap for an inter-electrode distance of 1.9mm. At high frequencies (103–106 Hz), the breakdown of even weakly polar liquids results from the intense heat release in the liquid and is characterized by a significant reduction in electric strength with increasing frequency. Table B.2 lists the effect of polarity on the breakdown of liquids for long discharge gaps used in high-voltage equipment. Table B.2. Effect of polarity on breakdown initiated in various liquids for a tip-plane electrode system at T = 293 K (From Ref. [8]). 196 Positive polarity always corresponds to the minimum electric strength and hence is most dangerous to insulation of high-voltage equipment. Only for inter-electrode distances of several tens of microns, the breakdown voltage of the majority of liquids for positive polarity of the tip electrode is higher than for negative one. In addition, the polarity effect is much more evident in liquids with high permittivity. For breakdown of liquids containing electronegative groups or molecules (for example, carbon tetrachloride, benzene chloride, etc.), the polarity effect is essentially nonexistent. From Table B.2, we can also see that, the addition of chlorinated hydrocarbons (the molecules of which possess considerable electron affinity) to transformer oil, whose breakdown is accompanied by a sizable polarity effect, eliminates almost completely the polarity effect. Chemical nature, composition and volume of liquids The establishment of a relation between the liquid electric strength and the atomicmolecular structure would allow one to predict the dielectric properties of liquids from the known physical and chemical constants and to seek for and to synthesize the liquid insulation as well as to use additives improving the dielectric properties of liquids. However, no reliable relations have been derived by the present time because of the influence of impurities of different types that are always present in the liquid, a great variety of processes that affect the liquid breakdown, and the lack of a well-developed theory of the liquid phase of matter. Under pulsed voltages, the effect of impurity on the breakdown decreases due to inertia of the secondary processes, but the results obtained allow one to establish only tendencies of changes of the electric strength for liquids distinguished by those or other physical and chemical properties. 197 Besides, it was demonstrated that rather inconsistent data on the influence of properties and structure of liquids on their electric strength were mostly due to difficulties in considering the influence of the electrode surface state. Under long-term voltage exposure, the electrical conductivity γ of liquids affects significantly their electric strength. An increase in γ reduces the electric field strength necessary for the implementation of the electrothermal breakdown mechanism. However there are contradictions indicating a complex character of the breakdown strength dependence on γ (it also depends on the field geometry and pulse polarity). For example, Figure B.7 shows the dependences of breakdown voltage of aqueous NaCl solution on γ for the nanosecond breakdown in a uniform (Figure B.7a) and nonuniform fields of the tip-plane electrodes (Figure B.7b). Figure B.7 (from Ref. [8]). Dependence of the electric strength of the NaCl aqueous solution on the electrical conduction in a uniform field at td = 70 ns and d = 0.02 cm (a) and in a non-uniform field at td = 90 ns and d = 0.015 cm (b) for −T +P (curve 1) and +T −P electrodes (curve 2). The working mechanism of various additives injected into liquid dielectrics to increase their electric strength is primary associated with the two effects: a) a decrease in the field nonuniformity in the insulation gap due to a local increase in the electrical conductivity, or to 198 polarization processes at the interface between the solid and liquid phases (when solid particles are introduced into a liquid) and b) the effect of additives on the behavior of charge carriers produced by emission and ionization. To reduce the influence on liquid dielectric breakdown of electrode microgeometry and processes adjacent to electrodes, it has been suggested that surface conducting layers be created whose electrical conductivity decreases smoothly with depth, and whose effective thickness is significantly greater than the size of micro-inhomogeneities, but less than the gap distance. If the voltage duration are not too short, the electric strength of the insulation gap is expected to increase due to the diminished effect of the near-electrode processes that initiate breakdown. Figure B.8a shows the behavior of the normalized electric strength E/E0 of water with βalanine as a function of the additive concentration (E and E0 denote the 50% breakdown strength of water with and without amino acid additives). The data were obtained for a high-voltage oblique-front pulse width of 5 μs, a distance between the plane electrodes of 1 cm, and areas of the stainless ferrite steel and aluminum electrodes of 30, 110, and 150 cm2. From Figure B.8a it can be seen that E/E0 is a complex function of amino acid concentration, with details determined by the electrode material. For the stainless ferrite steel electrodes, E/E0 = f(c) has a maximum at c = 0.03 mol/L equal to E/E0 = 1.33. For c ≥ 0.06 mol/L, the electric strength of water with the additive is the same as that of pure water. For the system with austenitic steel electrodes, E/E0 = f(c) has two maxima at c1 = 0.03 mol/L (E/E0 = 1.48) and c2 = 0.055 mol/L (E/E0 = 1.41). For aluminum electrodes, the injection of amino acids into water reduces its electric strength over the entire range of concentrations examined. An increase in the electric strength of water containing additives is accompanied by a decrease in the standard deviation σ of the breakdown field 199 strength. Minimum values of σ correspond to maximal values of breakdown electric field (Figure B.8b). Figure B.8 (from Ref. [8]). Dependences of the relative electric field strength (a) and standard deviation of the water breakdown field strength (b) as function of the β-alanine concentration for austenite (curve 1), ferrite stainless steel (curve 2) and aluminum electrodes (curve 3). The significant influence of the volume of liquid dielectric in a strong electric field on the electric strength results from the fact that the in the bulk of the liquid strongly affect the discharge initiation near the electrodes, and subsequent propagation within the gap. The relationship between electric strength and liquid volume depends heavily on the elemental composition of the liquid, the prevalence and nature of impurities, the discharge gap configuration, the electric field, and the exposure time of the liquid. In general, breakdown field strength was halved when the dielectric volume increased by two orders of magnitude. Experimental results have demonstrated that breakdown voltage increases by approximately 22% when the oil volume in a strong electric field doubles with electrode area remaining unchanged. 200 9 Recent Progress The main source of the literature is Proceedings of IEEE International Conference on Dielectric Liquids (1990-2005). Some papers were later published in IEEE Transaction on Dielectrics and Electrical Insulation from which more papers are chosen to review. The power frequency insulation breakdown phenomena in pure hydrocarbon liquids including straight, branched, and ring-type chemical structures with different electrode shapes and materials was investigated in [9]. The electric strength of n-pentane, n-hexane, n-heptane, benzene, toluene, xylene, and 2,2,4-trimethyl pentane was determined using brass, copper, and aluminum electrodes in sphere-plane, sphere-sphere, tip-plane, tip-sphere and tip-tip configurations. It was found that, n-hexane with copper sphere-plane arrangement yields maximum electric strength, while n-pentane with aluminum tip-tip arrangement yields minimum electric strength. Besides this result, the comparative study method applied in [9] also provided a good example for designers to obtain maximum breakdown strength when many options are available. In [10], the effect of forced flow velocity on the breakdown voltage/gap length characteristics of transformer oil was studied using a needle point and a mesh plane electrode system. The velocity of the axial (co-field) oil flow varied from 0 to 280 cm/s. For degassed oil there was a large increase in the breakdown voltage with increasing oil velocity for both voltage polarities. For O2- and SF6-saturated oils a similar increase in breakdown voltage was observed only with the point negative. With the point positive, velocities above 90 cm/s had no effect. Breakdown voltage versus gap length (1-12 mm) characteristics were obtained in [11] for transformer oil under uniform field. It was observed that, the breakdown voltage increases with 201 increasing oil gap spacing between electrodes, though the average breakdown field decreases. The breakdown voltage values are higher for aluminum electrodes than stainless steel. The breakdown voltage for dehydrated oil was improved by about 100% as compared with oil containing emulsion droplets of water by (0.2% by mass). Variation of breakdown strength with temperature is very sensitive between 20 and 40 oC (decrease by about 50%), implying that a cooling procedure could be effective in this case. Figure B.9 (from Ref. [12]). Breakdown electric field as a function of distance between electrodes with (a) different material pairs and (b) different impurity concentrations. It was shown in [12] that modification of interface properties, whether by electrode material or by introducing impurities, substantially changes the electric breakdown strength of the electrode-liquid system. As shown in Figure B.9(a), different combination of electrode materials results in different electric strength; in Figure B.9(b), when electron donor impurity concentration (butanol) is 5%, electric strength gains maximum improvement. 202 Theoretical research on the effect of molecular impurities on the development of ionization electron avalanche and on the electrical strength of atomic liquids (liquid Ar, Kr and Xe) was presented in [13]. The decrease of pre-breakdown voltage was predicted mainly due to more efficient vibration excitation of molecules by electron collisions. Another quantitative theoretical study [14] of the intrinsic dielectric strength of condensed helium under cryogenic temperatures applied the method of the electron kinetic Boltzmann equation to calculate the impact ionization coefficients and other related transport quantities, which can be further used to find the breakdown fields and the breakdown formation times. In [15], the field strength needed for runaway up to a self-sustaining discharge was calculated using an anti-bubble barrier model for various electrode surface roughnesses. Cathode surface roughness plays a significant destructive role in electric strength in the low temperature range 2.5-4.5 K. Using point-plane geometries, with gaps of 5 mm or larger, it was shown in [16] that typical transformer oils have higher breakdown voltages when the point is negative than when it is positive. Perfluorinated polyethers were found to produce opposite results when average gap size is 5 to 10 mm. For larger gaps the sequence was reversed again. The author of [17] conducted optical and statistical studies of electrical breakdown of n-hexane under a quasiuniform field of 0.9-3.5 MV/cm (the duration of voltage exposure ranges from 20 ns to 2 μs) with gaps 25-150 μm in length. It was established that increase in breakdown field with reduction in gap length takes place in the case of the bubble breakdown mechanism by reduction of the local electrical field near the cathode surface. Ref. [19] reported the effect of enforced cross-field flow on the variation of dc breakdown voltage for transformer oil and point-to-plane electrode geometry with gap length of 200-900 μm. It was shown that cross-field flow is more effective than co-field to increase the 203 breakdown voltage, whereas in the latter case only when the point is positive this effect is obvious. Barrier effect on the prebreakdown and breakdown phenomena in long oil gaps was investigated in [20]. The experimental setup is illustrated in Figure B.10(a). It was shown that the effectiveness of an insulating barrier, namely the ratio of the breakdown voltage of oil gaps in presence of barrier to that one without barrier, in a divergent field, is the higher when the barrier is placed near the sharp electrode (at 0 to 25% of the electrode gap), and when the polarity is positive. The results are indicated in Figure B.10(b). (a) (b) Figure B.10 (from Ref. [20]). (a) Scheme of the test cell; (b) 50% lightning impulse breakdown voltage vs. relative position (a1/a) of the barrier for a=50 mm. Performance of non-homogenous insulating oil mixtures under dc conditions was studied in [21], which concluded that mixtures have reduced breakdown strength than that of either of the two oils. In [22], the authors investigated breakdown characteristics of pressurized liquid nitrogen (LN2) over a very wide range of electrode size. Experimental results revealed that the breakdown mechanism changed from an area effect to a volume effect when increasing the 204 highly stressed liquid volume in LN2. Moreover, the contribution of area and volume effects to the breakdown strength in LN2 was discussed. The standard ac dielectric breakdown test result is generally used as one of the acceptance criteria for insulating oil and a maintenance tool for high-voltage power transformers in service. In [23], oil breakdown results were systematically evaluated and compared using ASTM and IEC standard procedures and varying many of the test parameters such as the shape and dimensions of the electrodes, the oil circulation, the voltage application procedure, etc. As shown in Figure B.11, testing procedures have strong influence on the results. Figure B.11 (from Ref. [23]). Influence of testing procedures on the breakdown behavior of in-service contaminated oil. The increase of the electric stress, in large high voltage dc filter capacitors manufactured with all polypropylene film dielectric impregnated with synthetic hydrocarbons, is limited due to the high dispersion of the values of the dc breakdown voltage. The paper [24] described the results obtained adding to the impregnating liquid a scavenger. The dc breakdown voltage dispersion is reduced. The capacitor dielectric stress is also increased. 205 The effect of co-field oil flow on the direct breakdown voltage in transformer oil using a point-to-plane electrode geometry for both polarities of the point was investigated in [25]. Tests were carried out on degassed oil, oil saturated with O2 and with N2 and oil with 1methylnaphthalene and dimethylaniline as additives. The oil flow velocity varied from 0 to 170 cm/s. For degassed oil, N2-saturated oil and oil with DMA as additive, the results show that for both point polarities the breakdown voltage increases with increasing oil velocity, attains a distinct maximum value at a certain velocity and then decreases for higher velocities. For O2saturated oil and oil with MN as additive the breakdown voltage increases with increasing flow velocity and attains a quasi-saturation value for velocities in the range 100-120 cm/s. With N2 and DMA, breakdown voltages were in general lower than those for degassed oil, where as with O2 and MN they were substantially higher. Cryogenic liquids are claimed to have a noteworthy impact on the concept of improved future power equipment. The low boiling temperature of liquid helium or liquid nitrogen offers the use of superconducting materials. On the other hand, the liquids seem to be interesting basic insulators with reasonable dielectric performance. Liquid nitrogen and helium are two common choices. Figure B.12 from [26] gives typical dielectric strength course of insulators with comparison with others (a) and long term degradation in ac breakdown strength (b). The experimental investigation in [27] showed the effect of electronegative dissolved gases on the conduction current level in transformer oil. The degassed mineral oil containing C8F18 gas exhibits a reduction in the conduction current levels than that of only mineral oil, and also the maximum stress reaches a higher threshold. The C8F16O/N2 mixture has this effect even stronger than C8F18. With a hydrostatic pressure, the effects can be further signified. 206 (a) (b) Figure B.12 (from Ref. [26]). (a) Typical dielectric strength course of insulators in insulation systems; (b) long term degradation in ac liquid breakdown strength. In [28], the authors made effort to evaluate linear alkyl benzene for a new kind of transformer oil. It was concluded that electrical, chemical and physical along with ageing characteristics of LAB are comparable to existent transformer oils (the dielectric strength of LAB is reported twice that of transformer oil). Effects of bubbles with and without dissolved SF6 gas on the ac and lightning impulse insulation characteristics of perfluorocarbon was studied in [29]. With the bubbles in perfluorocarbon liquid, breakdown phenomena related to bubbles crossing a uniform field gap studied. It was found that insulation strength with bubbles is remarkably lower than without bubbles under ac voltage, but not so remarkable under lightning impulse. Ref. [30] reported on measurements investigating the dielectric strength of insulating oil and from very low (-20°C) to increased temperature (+60°C). Different insulation structure models-board puncture and creepage-were stressed with 1 hour dc step-by-step voltage increase of reversed polarity each step, until breakdown. The impact of adhesives and their orientation 207 relative to the electric field was investigated. It was noted that at -20°C, the electric strength of oil becomes critically low. The effect of emulsion water in liquid hydrocarbons (benzene, toluene, ethyl benzene, pdiethylbenzene, cyclohexane, and heptane) on the conduction process has been studied in [31]. The content of water in the investigated liquids was changed from 0.1 % to 1.0 %, by weight and microemulsions of water in liquid hydrocarbons were produced ultrasonically. In general, conductivity monotonically increases when the concentration of emulsion water increases, but in case of water mixtures with benzene and toluene a deviation from this monotony was observed, as shown in Figure B.13. (a) (b) Figure B.13 (from Ref. [31]). Resistivity as a function of water content in (a) benzene and (b) toluene. In Ref. [32], the performance of ester and mineral oil/ester mixtures concerning the electric behavior was presented. The breakdown voltage of the mixtures is less temperaturedependent than that of the pure mineral oil. The reason is the difference in the water saturation 208 limit. It was suggested that, if the transformer usually operates at very low temperatures, the application of the mineral oil and ester liquid mixtures offers increased insulation reliability. The dielectric strength at low temperatures is higher than that for pure mineral oil. The efficiency of the hydration was checked using ester liquid as insulation or only as water carrier to fry the paper in a long or short time period. Investigations on the electrical strength properties of oil gaps were carried out with uniform electrical fields and electrode distances up to 30 mm [33]. Measurements were performed with alternating current (50 Hz), lightning impulses and switching impulses. It was shown that it is possible to minimize the dispersion to values of about 5 to 6 percent. The application of insulating liquids together with a solid insulant immersed therein is essential for some kinds of applications like power transformers. A dominant risk, reducing the strength of such insulations, is water, thus drying procedures are required to extend lifetime and operation reliability. Ref. [34] presented new systems, which perform a continuous desiccation of the insulating system of power transformers during service and are beneficial for insulating liquids as well as for solid insulations immersed therein. The requirements on the liquid part of the insulating system are not only the electric and dielectric performance but also the performance regarding environmental requirements and dehydration capability as well as low in flammability. It was reported in [35] that, the use of ester liquid Midel 7131, partly or totally replacing mineral oil, reduces the risk of environmental pollution, increases the lifetime of the component and reduces the fire risk. Some results concerning the electric and dielectric behavior of Midel 7131 is presented and pure Midel 7131 as well as mixtures with mineral oil fulfill the requirements on the electrical performance of liquid insulating materials. 209 Ref. [36] deals with breakdown voltage characteristics of saturated liquid helium, in the presence of a metallic particle in shape of needle or sphere to obtain insulation design data for the pool-cooled low temperature superconducting coil and to find the factors dominating the breakdown voltage. The main results are: 1) foreign particle in liquid helium causes a high stress field and the phase change of liquid helium and reduces the breakdown voltage by more than several tens of percents; 2) at higher pressures, breakdown voltage is improved due to inhibition of bubbles. Ref. [37] is aimed at the improvement of power transformers through the improvement of the characteristics of mineral oil by mixing this later with other insulating liquids for transformers namely silicon and synthetic ester oils. A comparison of breakdown voltage was presented in Figure B.14. This work gives prominence to the mixture mineral oil / 20% synthetic ester oil as a good compromise to get a liquid better than mineral oil alone. In that sense, it appears that this mixture could improve the power transformer insulation. The effect or ice on dc pre-breakdown events was investigated using a needle-to-plane electrode system in liquid nitrogen at 77.3 K in [38]. It was found that breakdown voltage may be raised due to the attachment of ice to the electrode. In [39], with respect to the electrical breakdown mechanism in superconducting coils with a finned wire under quenching conditions, the bubble dynamics and the correlation between bubble behavior and breakdown voltage characteristics are investigated using a plane-to-cylinder gap with/without triangular fins. The results shown in Figure B.15 indicate that the gradient force and Maxwell stress strongly affect the bubble dynamics and bubble shape in the gap. Especially the pronounced gradient force near the fin tip reduces the stable growth of bubble there. This results in a smaller effect of thermal bubble on the breakdown voltage, if the fins are formed to avoid electrically the appearance of bubble in the shortest gap region at higher applied voltages. 210 Figure B.14 (from Ref. [37]). Breakdown voltage evolution of oils and mixtures with 6 measurements. [Water content (ppm) / Pollution class (NAS 1638)]. (a) (b) Figure B.15 (from Ref. [39]). (a) Bubble distribution and dielectric behavior in three cylinder-to-plane gaps with different cylinder surface conditions near breakdown voltages; (b) Breakdown voltages of three cylinder-to-plane gaps with different cylinder surface conditions. 211 The lightning impulse breakdown characteristics of various combinations of insulation material in silicone oil for use in electric power apparatus were investigated in [40], with the aim of reducing the amount of oil required and thus the cost. Breakdown characteristics were investigated in a system in which insulating filler was mixed with silicone oil. The relation between the breakdown strength and the electric field strength was clarified. Based on the findings, optimum conditions for the use of silicone oil in electric power equipment are proposed. Recently ester oil dielectrics have been introduced as substitutes for mineral oil for use in power transformers. These oils have several advantages over other transformer oils as they are non-toxic, more biodegradable and less flammable. In [41] samples of one hundred ac breakdown voltages of esters and mineral oil are analyzed to compare their statistical distributions, in particular whether the lowest observed breakdown voltages are different. The results in Table B.3 indicate that these oils can be at least as capable as mineral oil for transformer insulation. Table B.3. Comparing withstand voltages of non-parametric and parametric methods (from Ref. [41]). 212 10. Some Concluding Remarks The electrical strength of all dielectric liquids depends on pressure, the dependence itself depending on the voltage duration, degree of liquid degassing, electrical conductivity and electrode configuration. However, an increase in pressure changes the conditions of gas formation, displaces the equilibrium between molecular dissolved gas and gas bubbles toward the former, reduces gas bubble size and increasing gas pressure inside the bubbles, thereby hindering the ionization processes. In this way, higher hydrostatic pressure can lead to an increase in the electrical strength. This can be regarded as the most straightforward way to increase the breakdown voltage of a liquid insulation. Interest in electrode coating, a well-known but seldom used method of increasing breakdown voltage of liquid insulation gaps, has significantly increased over the past few years. Data on the influence of electrode coatings on the electrical strength of gaps filled with liquids are inconsistent. Space charge control aims at reducing the electric field at electrodes by space charge injection. Qualitatively, space charge distortion of the electric field distribution between parallel plate electrodes with spacing d at voltage V so that the average electric field is E0=V/d. When no space charge exists, the electric field is uniform at E0. Unipolar positive or negative charge injection so that the electric field is reduced at the charge injecting electrode and enhanced at the non-charge injecting electrode. Bipolar homocharge injection so that the electric field is reduced at both electrodes and enhanced in the central region. Bipolar heterocharge distribution where the electric field is enhanced at both electrodes and depressed in the central region. We need to choose optimum metal/dielectric material combinations to achieve the bipolar homocharge injection and therefore increase electric breakdown strength, though the electric field is increased 213 in the center of the gap, but breakdown does not occur because the intrinsic strength of the dielectric in the volume is larger than at an interface where microasperities are often present. Electrodes of different metals showing differences in the magnitude and sign of the injected charge. In highly purified water stainless steel electrodes generally inject positive charge, aluminum injects negative charge, while brass can inject either positive or negative charge. Thus by appropriate choice of electrode material combinations and voltage polarity, it is possible to have bipolar homocharge liquid. Past work has shown that using water between a positive stainless steel electrode and a negative aluminum electrode resulted in homopolar charge injection from both electrodes that increased the electric breakdown strength in water by 40% over the opposite voltage polarity with no charge injection. Impurities, generally speaking, play a negative role in the breakdown strength of dielectric liquids. However, there are exceptions. The first example is additive to prevent the reduction in dielectric strength due to aging. Other work has demonstrated the paradoxical fact that conducting nanoparticle suspensions in transformer oil have superior positive electrical breakdown to that of pure oil while insulating nanoparticles offer no insulation advantage over pure oil. Electrical breakdown testing of magnetite nanofluid found that for positive streamers the breakdown voltage of the nanofluids were almost twice that of the base oils during lightning impulse tests. 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Sano, et al., “Effect of bubbles on breakdown strengths of perfluorocarbon liquid and the liquid with dissolved SF6,” Proceedings of 13th International Conference on Dielectric Liquids, pp. 525-528, 1999. [30] C. Krause and R. Woschitz, “The temperature dependence of the dielectric strength of transformer oil and pressboard insulation at HVDC polarity reversal stress,” Proceedings of 14th International Conference on Dielectric Liquids, pp. 182-185, 2002. [31] B. Dikarev, R. Romanets, V. Bolshakov, et al., “Influence of emulsion water on conduction in dielectric liquids,” Proceedings of 14th International Conference on Dielectric Liquids, pp. 199-202, 2002. [32] E. Gockenbach, and H. Borsi, “Performance and new application of ester liquids,” Proceedings of 14th International Conference on Dielectric Liquids, pp. 203-206, 2002. [33] W. Lick, and M. 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Bessede, “Improvement of power transformers by using mixtures of mineral oil with synthetic esters,” Proceedings of 15th International Conference on Dielectric Liquids, pp. 389-392, 26 June1 July 2005. [38] R. Hanaoka, R. Ishibashi, Y. Usui, et al., “Effect of electrode ice layer on prebreakdown current in liquid nitrogen,” IEEE Trans. Dielectr. Electr. Insul., 1 (4): 741-746, 1994. [39] M. Hara, Z. Wang and H. Saito, “Thermal bubble breakdown in liquid nitrogen under nonuniform fields,” IEEE Trans. Dielectr. Electr. Insul., 1 (4): 709-715, 1994. [40] H. Miyahara, A. Nakajima, and S. Yanabu, “Insulating system to reduce the amount of oil in electric power apparatus using silicone oil,” IEEE Trans. Dielectr. Electr. Insul., 15 (2): 533-539, 2008. [41] D. Martin and Z. D. Wang, “Statistical analysis of the ac breakdown voltages of ester based transformer oils,” IEEE Trans. Dielectr. Electr. Insul., 15 (4): 1044-1050, 2008. 217 218 C Pictures of the Kerr electro-optic measurement system As shown in Figure C.1, the small Kerr cell (6 inches tall and 8 inch diameter) was used for all of the propylene carbonate measurements at the beginning of the research project. The cell has a fixed rod in the bottom and moveable rod through the top that each electrode screwed onto, respectively. The top cover can be removed to fill or empty the cell with dielectric fluid. The high voltage cable is connected to the top moveable rod. The alignment of the electrodes to provide a parallel surface gap, in line electrodes, and secured electrodes that could not move when applying high voltage was a tedious process. Figure C.1. Small Kerr cell with optical components. 219 When conducting transformer oil measurements and breakdown tests the small Kerr cell quickly resulted in several problematic issues. When voltages were high enough to cause arcing, there was a high probability that arcing would happen between the electrode and the grounded test cell because the electrodes were near the sharp edged window viewing ports. The sharp edge causes a high electric field because the electric field lines want to terminate perpendicular to the conducting surface of the small test cell. The close proximity of the electrode ends causes nonuniform stressing of the glass windows. The small cell is more susceptible to changes in the ambient temperature and moisture because the volume contains a small amount of dielectric fluid causing difficulties in having uniform conditions for taking data. The processing and filtering of the oil requires the cell to be completely emptied, disassembled, cleaned, refilled, and reassembled. The small cell size and design make it difficult to add additional sensors. A larger existing chamber was modified into a larger Kerr cell. Further improvements were made by adding additional sensors and alignment components that were not able to be incorporated into the small Kerr cell. The large Kerr cell has an electrode holder that provided some difficulties in repeatable and accurate alignment of the gap spacing because the top moveable rod was difficult to secure and adjust accurately to provide the correct gap spacing. The placement of the electrode gap was horizontal resulting in contamination and suspended particles being trapped in the region of the gap. The large Kerr cell shown in Figure C.2 has a larger volume which allows for larger electrodes making the light path along the electrode surface longer, thereby accurately measuring the effect of electrical birefringence. The electrode ends are farther from the viewing window and the opening ports have more rounded edges. The changes in dielectric fluid condition due to ambient temperature and 220 moisture are less significant than in the small Kerr cell. The large cell can be heated and cooled via a circular pipe containing cooling fluid that spirals around the outside of the cell, but this functionality was not used. A filtering process was added to provide more uniform transformer oil conditions. The variable speed magnetic drive pump was used to circulate the oil. The circulating path is the pump intake to the cell bottom, 1µm filter, and pump outtake via flexible tubing to the top of the dielectric fluid level 180° across from the intake. The dielectric fluid can be filtered for long durations of time. A vacuum process was used to remove air bubbles suspended in the dielectric fluid before Kerr measurements were taken. The presence of a vacuum during the test allowed for any suspended particles formed after high voltage was applied to be removed from the liquid volume between the electrodes. The cell had two vertical rods inside the bottom that provided approximate alignment to the viewing windows. An electrode holder was designed and built to provide accurate and precise alignment of the electrodes. The holder design was an iterative process and the start and final holders are shown in Figure C.3. The holder could be adjusted manually, and placed the electrode gap vertical to allow for suspended particles and bubbles to be easily removed from the measurement region. The large size of the test cell can incorporate additional sensors such as temperature, conductivity, and filter oil flow. The disassembly and reassembly of the cell requires bolts on the top cover to be removed or replaced, respectively. Cell alignment can be difficult due to the size and weight when dielectric fluid is added. Further cell alignment is provided via a gantry plate and turn table. The gantry plate slides horizontally along two precision metal guide bars. The turn table between the cell and gantry plate permits the cell to be rotated. Various ports into the cell allow entry for additional sensors such as pressure, temperature, etc. 221 Figure C.2. Large Kerr cell with utility grade capacitor used for substation power factor correction. Figure C.3. Electrode holder (beginning design) and electrode module (final design). 222 A properly conditioned dielectric fluid is one main requirement for repeatable and reliable Kerr electro-optic measurements. This includes fluid filtering, circulation, and if needed temperature and moisture control. In this setup fine-tuned temperature and moisture control was not needed. A flexible input and output pipe circulate the fluid in the cell which can be manually directed between the electrode gap to clear any particles that may be trapped. The oil is continually run through a McMaster-Carr standard one cartridge filter (Model: 44185K65) with canister filter (Model: 44185K41) rating of 3µm to clear any contamination particles that were suspended in the fluid or introduced via various means. The filter has a gauge (Model: 44185K11) indicator to show when the filter needs replacement. The filter and pump are shown in Figure 9. The pump is a variable speed magnetic gear pump drive from Cole-Palmer with an inlet and outlet port of ¼ inch. Two control valves are used to isolate the pump, filter, and tubes from the cell. This provides easier replacement of oil conditioning equipment, filling or emptying of fluid. Figure C.4. Filter canister (3 µm filter rating) and variable speed gear pump drive for oil filtering and circulation. 223 224 D List of publications from thesis research • X. Zhang, J. K. Nowocin, and M. Zahn (2012), “Effects of AC Modulation Frequency and Amplitude on Kerr Electro-Optic Field Mapping Measurements in Transformer Oil”, in Annual Report of CEIDP, Montreal, Canada, pp. 700-704. • X. Zhang, J. K. Nowocin, and M. Zahn (2013a), “Evaluating the Reliability and Sensitivity of the Kerr Electro-Optic Field Mapping Measurements with High-Voltage Pulsed Transformer Oil”, Appl. Phys. Lett. 103, 082903. • X. Zhang, J. K. Nowocin, and M. Zahn (2013b), “Experimental Determination of the Valid Time Range for Kerr Electro-Optic Measurements in Transformer Oil Stressed by High-Voltage Pulses”, in Annual Report of CEIDP, Shenzhen, China, pp. 522-6. • X. Zhang and M. Zahn (2013), “Kerr Electro-optic Field Mapping Study of the Effect of Charge Injection on the Impulse Breakdown Strength of Transformer Oil”, Appl. Phys. Lett. 103, 162906. • X. Zhang and M. Zahn (2014a), “Fractal-Like Charge Injection Kinetics in Transformer Oil Stressed by High Voltage Pulses”, Appl. Phys. Lett. 104, 162901. • X. Zhang and M. Zahn (2014b), “Electro-optic Precursors of Critical Transitions in Dielectric Liquids”, Appl. Phys. Lett. 104, 052914. • X. Zhang (2014), “Electro-Optic Signatures of Turbulent Electroconvection in Dielectric Liquids”, accepted to publish in Appl. Phys. Lett. 225