RTP CRYSTALS FOR ELECTRO-OPTIC Q-SWITCHING M. Rotha, E. Samokaa, E. Mojaeva and M. Tseitlinb a Faculty of Science, The Hebrew University of Jerusalem, Jerusalem 91904, Israel b Research Institute, The College of Judea and Samaria, Ariel 444837, Israel Abstract. The wavelength dependencies of half-wave voltages for both X- and Y-oriented thermally compensated double-crystal RTP (RbTiOPO4) Q-switches have been determined by a common polarized optics technique. The dispersion of the respective electro-optic coefficients has been deduced from these results and compared with the existing data. Variation of the extinction ratios of the crystals in different geometries have been studied as a function of compositional gradients developing in the crystals during growth, parallelism of the optical elements and the wavelength used. The results show that the extinction ratio of such crystal is extremely sensitive to these parameters. 1. Introduction A new generation of oxide crystals is emerging for electro-optic Q-switching [1], or for high pulse power laser operation. As opposed to the acousto-optic Qswitches, where the overall turn-off time is limited by the sound wave transit duration (110-200 ns/mm) across the beam diameter, electro-optic devices offer a shorter than 10 ns response [2] needed for minimum loss in high-gain and high repetition rate solid state lasers. Better than 200:1 extinction ratios allow the electro-optic crystals to provide good hold-off, in contrast to about 40% single pass dynamic loss [3] with acousto-optic devices hindering the use of the latter in high gain lasers. Convenient electro-optic Q-switching can be achieved by amplitude or phase modulation in crystals due to optical distortion induced by an external electric field, namely employing the electro-optic effect [4]. Among the existing useful electro-optic crystals, such as the traditional DKDP [3] and lithium niobate [5] and the newer BBO [6] and langasite-structure [7] materials, the RTP (RbTiOPO4) crystal stands out in its ability to achieve amplitude modulation at extremely high frequencies, or repetition rates, of up to 1 MHz [8-10]. RTP belongs to the KTP(KTiOPO4)-family of ferroelectric optical crystals, but embodies a number of advantages over KTP. It has larger electro-optic coefficients and lower half-wave voltage [11], twice as high optical damage threshold (ca. 1.8 GW/cm2 for 10 ns pulses at 1.064 mm), and crystals with as-grown electrical resistivity > 1010 cm can be readily obtained. High resistivity RTP with proper choice of the evaporated electrode materials is not electrochromic. Excellent thermal stability in the 25-125°C temperature range has been reported for a couple of 11 mm long properly matched RTP crystals (thermally compensated scheme [8]), and their extinction ratio or the ratio of intensities of light passing through two polarizers with their axes oriented parallel and perpendicular to the beam polarization plane, can be as high as 800:1 [12]. However, the extinction ratio is closely related to the variation of the birefringence, n, or to the crystal optical uniformity across the crystal aperture. The latter depends directly on the compositional homogeneity of as-grown crystals. We have reported recently [13] that RTP crystals grown from self-fluxes undergo the ferroelectric phase transition in a relatively wide temperature range, from 770 to 202 800°C (Curie temperature, Tc), depending on the flux chemical composition in terms of the [Rb]/[P] atomic ratio. The actual Tc values are defined by the rubidium stoichiometry in the crystal, similarly to potassium stoichiometry in KTP [14], and they serve as a good relative measure of the compositional variation in large RTP crystals from the seed area to the periphery. Moreover, unlike KTP, nominally pure RTP crystals exhibit different Tc values for different growth sectors, even when solidified simultaneously. The questions of tolerance of the optical properties with respect to the compositional variations and the geometry of RTP electro-optic elements have to be elucidated. In the present work, we analyze and determine experimentally some key parameters important for the RTP operation as a thermally compensated doublecrystal electro-optic Q-switch, such as the half-wave voltage and effective electrooptic coefficients. Their dispersions for both X- and Y-cut crystal configurations are explored in a broad spectral range. The main factors influencing the extinction ratio are treated theoretically, and initial quantitative estimates with respect to the growthinduced optical nonuniformity are made. The influence of the optical element parallelism on the extinction ratio of the double-crystal design is discussed as well. 2. RTP Pockels cell Most common electro-optic Q-switching is based upon the rotation of polarized light by the linear electro-optic, or Pockels, effect in crystals lacking a center of symmetry, such as the ferroelectric RTP crystal. In the linear effect, the applied electric field causes a change in optical anisotropy of a birefringent crystal characterized by two orthogonal directions (fast and slow axes) with different indices of refraction, nf and ns, inducing a phase retardation = (2 l/)n, where n = nf – ns is the birefringence, l is the crystal length and is the wavelength of light. An incident plane-polarized beam (at 45° to the slow and fast axes) will split into two components traveling at different velocities and, upon traversing the crystal, will turn into an elliptical, circular or linearly polarized beam depending on the field magnitude [3]. The latter case corresponds to the more commonly employed 'half-wave' light intensity retardation. Hereby, the crystal is placed between two crossed polarizers, and in the 'light-pulse-on' configuration (no voltage applied) maximum light extinction is achieved. With the half-voltage (V) on, a 90° rotation of the linear polarization is caused at each pass of the beam through the crystal, and the light transmission given by [2] T ( I o / I i ) sin 2 ( / 2) (1) is maximal if (Io and Ii are the output and input light intensities respectively). When the light beam is directed off the optical axes, comprises also the natural (static) birefringence of the crystal, which is very sensitive to temperature changes. In order to achieve thermal stability of the Pockels cell operation, double-crystal compensated designs have been suggested for the biaxial KTP crystal [15] holding also for RTP. 203 (a) (b) -V -V Y +V +V Z X +V Z 45° +V Z 45° X -V Z Y Y -V Light polarization X Light polarization Fig. 1: Thermally compensated Q-switch designs for Y-cut (a) and X-cut pairs of RTP crystals. Figure 1 shows two configurations of Pockels cells utilizing double-crystal RTP layouts for plain-polarized light, at 45° to the Z,X or Y,Z axes, propagating along the Y- or X-direction respectively. For configuration (a), the phase retardation contributed by each crystal is given by [16] 3 l nz rc1V , d 2 3 l 2 l (nx nz ) nz rc1V , d 1 2 l ( nz nx ) (2) where rc1 = r33 – (nx/nz)3r13 is the corresponding effective electro-optic coefficient, V is the voltage across the electrodes (Z-direction) and d is the distance between electrodes. If the refractive indices and dimensions of each of the crystals are identical, the half-wave voltage can be derived by putting = 1 + 2 = : d V . 3 2rc1nz l (3) A similar relation can be given for a pair of X-cut RTP crystals, but rc1 must be replaced by rc2 = r33 – (ny/nz)3r23. Apparently, thinner and longer crystals are needed for reducing the half-wave voltage. 3. Experimental RTP crystals were grown by the top-seeded solution growth (TSSG) method with pulling on either X- or Y-oriented seeds from the R6 (Rb6P4O13) self-flux [13]. RTP solutions of desirable concentrations were prepared by reacting the Aldrich 3N purity TiO2, Rb2CO3 and Merck (Suprapur) NH4H2PO4 and (NH4)2HPO4 in appropriate proportions. The charges were loaded into 200 to 1000 ml Pt crucibles and subjected to 24 hours soaking through homogenization aided by a Pt stirrer prior to crystal growth. The crucibles were mounted in a custom-made resistance furnace with a long hot zone allowing to obtain a quite uniform temperature distribution with a gradient not exceeding 2°C in the solution. The pulling/rotation mechanisms and the online temperature and weight control were realized using the “Ariel-1” crystal growth system developed by Raicol Crystals Ltd. The seed rotation rates varied from 70 rpm to 20 rpm at different stages of growth. Variable pulling rates, from 0.02 to 1 mm/day were employed. Fine adjustment of the seeding temperature was achieved by repeated seeding with the seed-solution contact control using a thermoelectric circuit. The general temperature range for growth of RTP crystals from different self-fluxes 204 was 980-880°C, while the temperature lowering rates changed from 0.5 to 3°C/day. As a result, RTP crystals of 506050 mm3 dimensions along the X, Y and Z axis and weighing up to 450 g could be routinely obtained. Both X- and Y-cut crystal elements with optically polished faces were prepared for half-wave voltage measurements. Their typical dimensions were 4420 mm3, and the relatively large aspect ratio ([r]/[l] 1/5) was chosen in order to reduce the operating voltage. A custom made DC 5 kV power supply was used to apply variable voltage to the titanium electrodes evaporated on the RTP crystal Z-surfaces. The crystal was placed between crossed polarizers and irradiated with lasers of seven different wavelengths, namely: 473 nm (LaserCompact LCS-DTL-166QA DPSS laser doubled with a Raicol PPKTP elemnt), 532 nm (LaserCompact LCS-DTL-112QT DPSS laser), 633 nm (He-Ne laser), 946 nm (LaserCompact LCS-DTL-166QA DPSS laser), 1064 nm (LaserCompact LCS-DTL-112QT DPSS laser without a frequency doubling element), 1572 nm (obtained by OPO with the LAGRAN LTI-245 flashlamp pumped Nd:YAG laser and a Raicol KTP noncritically phase-matched element) and 2 (dedicated Tm:YAG DPSS laser [17]). Various Ophir Optronics power meters were employed for measuring the transmitted light intensity. Voltage was initially applied to the crystal to obtain complete light extinction. The polarizers were then aligned in parallel for maximum transmission, and the voltage was further raised until full extinction was achieved again. The difference between the two voltage levels was adopted as the half-wave voltage value for a crystal with the specific geometry used. 4. Results and Discussion 4.1 Half-wave voltage and electro-optic coefficients One of the most significant operational parameters of the electro-optic Qswitch is the maximum voltage that has to be applied. Despite the voltage limitations of power supplies and drivers used in the Q-switch system, lower voltage also reduces the detrimental leakage currents across the crystal and electrochromism [15]. According to eq. (3), one way of decreasing V, at a given wavelength, is reducing the aspect ratio (d/l), the other is employing a configuration with a larger effective electro-optic coefficient. Both in KTP [16] and RTP [12], the reported rc1 values are on the average 20% higher than those of rc2, implying that Y-cut RTP crystals are advantageous in terms of lower half-wave voltages. We have performed a detailed series of V measurements for both X- and Y-cut RTP crystals at seven different wavelengths (see Experimental), recalculated the experimental values for d = l (cubic crystal geometry), and the results are presented in Figure 2. 35 12000 8000 rc (pm/V) Half-wave voltage (Volts) 40 X-direction V = 9.3512λ - 2009.8 l =d 16000 Y-direction V = 8.0169λ - 1902.9 l=d 4000 30 25 20 15 0 0 500 1000 1500 2000 2500 0 500 1000 1500 Wavelength (nm) Wavelength (nm) 205 2000 2500 Fig. 3: Comparison of the -dispersion of rc1 (squares) and rc2 (triangles) effective electrooptic coefficients for Y- and X-cut RTP crystals respectively. Fig. 2: Wavelength dependencies of half-wave voltages of X-cut (upper slope) and Y-cut (lower slope) RTP crystals. The results show that Y-cut crystals indeed exhibit lower half-wave voltages at all wavelengths examined. Even at 2 , a 20 mm long RTP crystal may have a 6 mm aperture with a still reasonable V value. Linear dependencies have been obtained for both X- and Y-cut crystals, and the half-wave voltages can be easily calculated for any wavelength from the slopes (see boxes of Figure 2). Although, from eq. (3), V is proportional to , the linear dependences have not been expected a priori, in view of the existing dispersions in the refractive indices and electro-optic coefficients [18]. In fact, with the known -dispersion of the RTP refractive indices [19], the dispersion of rc1 and rc2 can be now calculated from the data of Figure 2. The results are depicted in Figure 3, and they represent the unclamped (constant stress) coefficients [18], rcT1 and rcT2 , since the measurements have been performed under DC voltage. The overall rc dispersion behavior is similar to KTP and other electro-optic crystals [18], but our measurements have been performed in a slightly broader spectral range, showing that in the near IR (above 1 ) the variation of electro-optic coefficients in RTP is insignificant. The fact of rc2 being about 20% smaller than rc1 emphasizes again the advantage of using Y-cut crystals, especially at longer wavelengths where the halfwave voltages are larger. 4.2 Extinction ratio One important performance parameter for an electro-optic Q-switch is the extinction ratio, ER, defined as the ratio of the transmission when the device is fully open (parallel polarizers) to the transmission when the device is fully closed (crossed polarizers), or sin 2 2 2 . ER 2 sin 2 (4) A high value of the extinction ratio is desirable because it determines the maximum contrast (ratio of light intensities at crossed polarizers with and without V). In practice there is always some light leakage, and the minimum transmission never reaches zero. Yet, commercial Q-switches can have excellent extinction ratios in excess of 1000, when the phase retardation is mainly due to the polarizing optics rather than to the electro-optic crystal. An ideal crystal employed for broad beam operation must have a high transverse optical uniformity. This can be largely achieved with an X-cut RTP crystal, since when grown in the X-direction the latter develops a large flat (100) facet [13], and the natural birefringence n = nz – ny const across the Pockels cell element face perpendicular to the light propagation direction. In reality, some optical nonuniformity is still induced by the point and line defects as well as thermomechanical stresses inherently present in crystals. However, the situation is essentially changed when Y-cut RTP crystals have to be used for their larger rc1 values. The Y-face embodies material layers that crystallize at different times, and a gradual variation of the transverse birefringence is expected due to compositional changes [13]. We assume linear variations of the refractive indices across the crystal 206 aperture, in similarity with the experimental data on KTP [20]. The transverse phase retardation for a beam propagating perpendicularly to the X-Z crystal plane is then expressed by 2 l (5) n z grad(n) , where n = nz – nx, while the gradient of the refractive indices along one of the two axes is known to be negligible, based on our experimental observations, depending on the crystal growth sector the sample is cut from. n at the center of the crystal can be compensated to zero, either thermally or using a phase plate, so the normalized transmission along the aperture d, for the crossed polarizers configuration (eq. (1)) can be calculated through the following integration: 1 0.5 d l T sin 2 z grad(n) dz. d 0.5 d (6) For the case of polarizers aligned in parallel, the argument under the sine function is ( +/2). After replacing the numerator and denominator in eq. (4) with the appropriate integrals of the eq. (6) type, we obtain ER = 12/2, where = [·l·d·grad(n)]/, (7) provided that < 1 – condition always met for a few mm to cm sized crystals and grad(n) ~ (1-2)105 cm1. Although the measured grad(n) in KTP [20] is of the order of 104 cm1, we presume that smaller compositional changes in RTP manifested by a more moderate variation of the Tc values [13,14] justifies the one order of magnitude smaller assessment of the refractive index gradient. Figure 4 shows the extinction ratio as a function of the crystal length at four different values of grad(n) for d = 5 mm and = 1064 nm. Extinction Ratio 2000 grad(Δn )=1.25*10^-5(cm^-1) 1500 grad(Δn)=1.5*10^-5(cm^- 1000 grad(Δn )=1.75*10^-5(cm^-1) 500 grad(Δn )=2.0*10^-5(cm^-1) 0 0.4 0.5 0.6 0.7 0.8 0.9 1 Length (cm) Fig. 4: Extinction ratio dependence on crystal length at four different values of transverse refractive index gradients for = 1064 nm (d = 5 mm). The sample curves of Figure 4 show that if the transverse gradient of refractive indices is kept smaller than 2105 cm1, even a 10 mm long crystal (with an aperture of 5 mm) yields a reasonably high extinction ratio of > 100:1. Shorter crystals are obviously better in terms of the ER, but a trade-off between high ER and low V (see Figure 2) has to be made. At longer wavelengths, say for the 2 Tm:YAG laser, the extinction ratio is substantially higher, since it scales as the square of the wavelength. 207 Naturally, factors other than the gradient of refractive indices difference may affect the extinction ratio. One of them is the lack of parallelism between the front and rear faces of the crystal. If the angle between the faces is , for an optically uniform crystal (n = const), the extinction ratio can be calculated using eq. (7) with = [·d·n·tan]/. (8) Adopting the typical commercial tolerance of = 10 arc sec, n = nz – nx = 0.086 at 1064 nm for RTP and d = 5 mm, we calculate ER 3170. This is a large number, well in excess of the ER values of Figure 4, implying that the practically achievable small nonparallelism may degrade the extinction ratio of the RTP crystals only for nonrealistically large apertures or at short wavelengths, although even near the RTP cutoff wavelength of 400 nm the extinction ratio due to nonparallelism is ~ 500. 5. Summary To summarize the above, a number of parameters important for Q-switching operation of RTP electro-optic crystals have been evaluated. The half-wave voltages of both X- and Y-cut RTP crystals have been determined experimentally in a wide spectral range, from below 0.5 to 2 . Y-cut crystals require an about 20% lower halfwave voltage (applied in the Z-direction) at any wavelength, which makes the single or double-crystal RTP Q-switch design with light propagating along the Y-direction of great advantage. However, our numerical calculations show that the appreciably lower transverse optical uniformity of Y-cut crystals limits their application to smaller apertures of 4-5 mm, if extinction ratios in excess of > 100:1 are required at reasonably low half-wave voltages. Our calculations also show that the practically achievable high parallelism of the crystal front and rear surfaces excludes nonparallelism as a tangible factor contributing to the phase retardation. 1. 2. 3. 4. 5. 6. 7. 8. 9. References M. Roth, M. Tseitlin and N. Angert, N. "Oxide Crystals for Electro-Optic QSwitching of Lasers", Glass Phys. Chem. 31, 86-95 (2005). A. Yariv, Quantum Electronics, ch. 14, Wiley and Sons, New York (1989). W. Koechner, Solid State Laser Engineering, ch. 8, Springer-Verlag, Berlin, 1996. A. Yariv and P. Yeh, Optical waves in Crystals, ch. 7, Wiley and Sons, New York (1984). X.D. Wang, P. Basseras, R.J. Dwayne Miller, J. Sweetser and I.A. Walmsley, "Regenerative pulse amplification in the 10 kHz range", Opt. Lett. 15, 839-841, 1990. G.D. Goodno, Z. Guo, R.J.D. Miller, J.W. Montgomery, S.R. Adhav and R.S. Adhav, "Investigation of -BaB2O4 as a Q switch for high power applications", Appl. Phys. Lett. 66, 1575-1577 (1995). B.H.T. Chai, A.N.P. Bustamante and M.C. Chou, "A new class of ordered langasite structure compounds", Proc. 54th IEEE Frequency Control Symposium, 163-168, Kansas City, MO (2000). E. Lebiush, R. Lavi, Y. Tsuk, N. Angert, A. Gachechiladze, M. Tseitlin, A. Zharov and M. Roth, "RTP as a Q-switch for High Repetition Rate Application", OSA Trends in Optics and Photonics Series 34, 63-65 (2000). S. Pearce and C.L.M. Ireland, "Performance of a CW pumped Nd:YVO4 amplifier with kHz pulses", Optics & Laser Techn. 35, 375-379 (2003). 208 10. 11. 12. 13. 14. 15. 16. 17. 18. 19. 20. J. Kleinbauer, R. Knappe and R. Wallenstein, "13-W picosecond Nd:GdVO4 regenerative amplifier with 200-kHz repetition rate", Appl. Phys. B 81, 163166, 2005. M. Roth, N. Angert, M. Tseitlin, G. Wang, T.P.J. Han, H.G. Gallagher, N.I. Leonyuk, E.V. Koporulina, S.N. Barilo and L.A. Kurnevich, "Recent Developments in Crystal Growth and Characterization of Nonlinear Optical Borate and Phosphate Materials", Proc. 3rd Int. Conf. Single Crystal Growth, Strength Problems and Heat and Mass Transfer, ed. V.P. Ginkin, V. 2, 416-426, Obninsk (2000). M. Roth, N. Angert and M. Tseitlin, "PotassiumTitanyl Phosphate (KTP) – an Oxide of Choice for Nonlinear Optical and Electro-optic Applications",Proc. 2nd Isr.-Russ. Workshop on the Optimization of Composition, Structure and Properties of Metals, Oxides, Composites, Nano- and Amorphous Materials, eds. M. Zinigrad and E.A. Pastukhov, 223-235, Ural Branch of RAS, Jerusalem (2003). M. Roth, N. Angert , M. Tseitlin, G. Schwarzman and A. Zharov. "Ferroelectric phase transition temperatures of self-flux-grown RbTiOPO4 crystals", Opt. Mater. 26, 465-470 (2004). N. Angert, M. Tseltlin, E. Yashchin and M. Roth, "Ferroelectric Phase Transition Temperatures of KTiOPO4 Crystals Grown from Self-fluxes", Appl. Phys. Lett. 67, 1941-1943 (1995). C.A. Ebbers and S.P. Velsko, "High average power KTiOPO4 electro-optic Qswitch", Appl. Phys. Lett. 67, 593-595 (1995). X.D. Wang, P. Basseras, R.J.Dwane Miller and H. Vanherzeele, "Investigation of KTiOPO4 as an electro-optic amplitude modulator", Appl. Phys. Lett. 59, 519-521 (1991). S. Goldring, E. Lebiush and R. Lavi, "RTP Q-switched 2-micron Tm:YAG laser", Proceedings of SPIE 4630, 13-16 (2002). M. Abarkan, J.P. Salvestrini, M.D. Fontana and M. Aillerie, "Frequency and wavelength dependencies of electro-optic coefficients in inorganic crystals", Appl. Phys. B 76, 765-769 (2003). L.K. Cheng, L.T. Cheng, J. Galperin, P.A. Morris Hotsenpiller and J.D. Bierlein, "Crystal growth and characterization of KTiOPO4 isomorphs from the self-fluxes", J. Crystal Growth 137, 107-115 (1994). A. Miyamoto, Y. Mori, Y. Okada, T. Sasaki and S. Nakai, "Refractive index and lattice constant variation in flux grown KTP crystals", J. Crystal Growth 156, 303-306 (1995). 209