Effect of low frequency voltage waveform on plasma uniformity in a dual-frequency capacitively coupled plasma Cite as: J. Vac. Sci. Technol. B 40, 032202 (2022); https://doi.org/10.1116/6.0001732 Submitted: 30 December 2021 • Accepted: 15 March 2022 • Published Online: 04 April 2022 Shahid Rauf, Peng Tian, Jason Kenney, et al. COLLECTIONS Paper published as part of the special topic on Plasma Processing for Advanced Microelectronics ARTICLES YOU MAY BE INTERESTED IN Electron dynamics in low pressure capacitively coupled radio frequency discharges Journal of Applied Physics 127, 181101 (2020); https://doi.org/10.1063/5.0003114 Focus ring geometry influence on wafer edge voltage distribution for plasma processes Journal of Vacuum Science & Technology A 39, 043006 (2021); https:// doi.org/10.1116/6.0000981 Overview of atomic layer etching in the semiconductor industry Journal of Vacuum Science & Technology A 33, 020802 (2015); https:// doi.org/10.1116/1.4913379 J. Vac. Sci. Technol. B 40, 032202 (2022); https://doi.org/10.1116/6.0001732 © 2022 Author(s). 40, 032202 ARTICLE avs.scitation.org/journal/jvb Effect of low frequency voltage waveform on plasma uniformity in a dual-frequency capacitively coupled plasma Cite as: J. Vac. Sci. Technol. B 40, 032202 (2022); doi: 10.1116/6.0001732 Submitted: 30 December 2021 · Accepted: 15 March 2022 · Published Online: 4 April 2022 Shahid Rauf,a) View Online Export Citation CrossMark Peng Tian, Jason Kenney, and Leonid Dorf AFFILIATIONS Applied Materials, Inc., 1140 E. Arques Ave., Sunnyvale, California 94085 Note: This paper is a part of the Special Topic Collection on Plasma Processing for Advanced Microelectronics. a) Author to whom correspondence should be addressed: shahid_rauf@amat.com ABSTRACT In a dual-frequency capacitively coupled plasma (CCP) with disparate frequencies, the low frequency (LF) voltage usually has a strong influence on the ion energy distribution function (IEDF) but contributes less to plasma generation. It is well-known that rectangular LF voltage waveform with a small positive period yields a narrow, nearly monoenergetic IEDF. This paper focuses on the effect of the LF voltage waveform on plasma uniformity in a low-pressure dual-frequency (40 + 0.8 MHz) CCP. A two-dimensional particle-in-cell model is used for this investigation, and the effect of LF voltage amplitude on plasma uniformity is investigated for sinusoidal and rectangular voltage waveforms. When the LF voltage is low, the peak in plasma density is at the chamber center due to ample diffusion at the low pressure considered (20 mTorr) and higher losses to the chamber walls. As the LF voltage is increased, the sheath gets thicker at the powered electrode and charged species densities decrease for a constant 40 MHz voltage. The plasma profile, however, evolves differently for the two LF voltage waveforms. With sinusoidal LF voltage, the plasma spreads out between the electrodes. On the other hand, with rectangular LF voltage waveform, the plasma splits into two regions: a density peak at the chamber center and another peak near the electrode edge. This doublepeaked density profile with a rectangular wave can be attributed to the location and timing of plasma generation. 40 MHz produces plasma most efficiently when the LF rectangular wave is positive and the sheath at the powered electrode is thin (frequency coupling). This plasma is produced uniformly between the electrodes, but only for a short period. When the LF voltage becomes negative, the sheath expands at the powered electrode and the plasma is produced near the electrode edge where the sheath is thinner and the electric field is stronger. Published under an exclusive license by the AVS. https://doi.org/10.1116/6.0001732 I. INTRODUCTION Low-pressure multifrequency capacitively coupled plasmas (CCPs)1 are used for many plasma processing applications in the semiconductor industry. A common methodology is to use two disparate frequencies where the higher frequency primarily contributes to plasma production while the low frequency (LF) is used to control the ion energy distribution function (IEDF).2,3 Considerable attention has been paid recently to the use of nonsinusoidal LF waveforms to control the IEDF. In particular, it has been demonstrated that rectangular voltage waveform with a small positive period yields a narrow, nearly monoenergetic IEDF.4 Even though the LF source might not significantly contribute to plasma production directly, it has considerable influence on the plasma J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS through the control of the sheaths in a CCP. The goal of this article is to use a two-dimensional cylindrical geometry particle-in-cell (PIC) plasma model to understand how the LF waveform influences the plasma spatial properties in an axisymmetric cylindrical plasma reactor. PIC model has been found necessary for this study as electron kinetic effects, which are important in all low-pressure CCPs, become even more significant for rectangular voltage waveform with sharp changes in voltage. There is considerable literature on the design and modeling of multifrequency CCPs as well as their PIC modeling. We limit our literature review in this article to two pertinent topics: the use of nonsinusoidal voltage waveforms to control the IEDF and 2D PIC modeling of CCPs. The early work on the use of nonsinusoidal voltage waveforms to control the IEDF was done in inductively 40, 032202-1 ARTICLE coupled plasmas.4,5 Wang and Wendt4 experimentally demonstrated that a rectangular voltage waveform can be used to get a narrow IEDF. They also showed how these IEDFs can be used to control selectivity during plasma etching,6 a feature that is particularly helpful for atomic layer etching.7 Nonsinusoidal voltage waveforms can be obtained by combining multiple harmonics. Czarnetzki et al.8 described this approach in the context of the electrical asymmetry effect in CCPs and showed that multiple harmonics could be used to obtain a narrow IEDF. Schüngel et al.9 elaborated on the method to generate single peak ion flux energy distribution using waveform tailoring. Delattre et al.10 presented detailed diagnostics and modeling results to examine the effect of waveform tailoring on Ar plasma characteristics at low pressures. Lafleur’s review on tailored waveform excitation of CCPs (Ref. 11) excellently summarizes the use of waveforms generated using a combination of harmonics to control plasma properties, in particular the DC self-bias. Franek et al.12 described a new radio frequency (RF) power supply and impedance matching method suitable for customized voltage waveforms. Schmidt et al.13 and Wang et al.14 further developed multifrequency matchboxes based on series and parallel LC circuits that are suitable for waveform tailoring. Brandt et al.15,16 experimentally and numerically investigated electron heating in CF4 and Ar/CF4 CCP discharges excited using multiple consecutive harmonics of 13.56 MHz. Derszi et al.17 investigated power coupling in O2 CCP discharge generated using a combination of harmonics. Hartmann et al.18 have recently modeled CCPs with high voltage tailored voltages and shown that tailored waveforms can also be used to control the electron velocity distribution, especially at high energies. These energetic electrons generated during electric field reversal in the sheath can be useful for high aspect ratio dielectric etching, as discussed by Krüger et al.19,20 Many previous studies have addressed 2D PIC modeling of CCPs. Kim et al.21 modeled high-pressure CCPs in Cartesian geometry highlighting the plasma nonuniformities at the electrode edges. 2D simulations are more challenging in cylindrical geometry due to small differential volume and consequent large statistical error near the axis. The early 2D cylindrical-geometry model of dual-frequency CCP by Wakayama and Nanbu22 is noteworthy in this regard. Their published results illustrate the effect of interelectrode spacing on plasma uniformity, especially near the axis. Wang et al.23–25 published a series of articles about a 2D implicit PIC model of CCPs. They examined issues related to plasma uniformity and compared PIC and fluid plasma modeling results. Rauf26 described a 2D PIC model for an axisymmetric cylindrical chamber, validated modeling results using experiments and examined kinetic effects influencing plasma transport. Wang et al.27–29 used a 2D PIC model to examine the electric asymmetry effect in a geometrically asymmetric CCP reactor and investigated the effect of plasma reactor geometrical asymmetry. This article is organized in the following manner. The computational model is described in Sec. II. Modeling results are discussed in Sec. III, and Sec. IV includes a summary. II. COMPUTATIONAL MODEL The investigation in this article has been conducted using a modified version of the plasma model described in Ref. 26. In this J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS avs.scitation.org/journal/jvb model, charged species are simulated using PIC while neutral species are treated as a fluid. To briefly recap the modeling methodology, we start with assumed initial densities, connect appropriate RF sources to the electrodes, and simulate the evolution of charged and neutral species until all major quantities converge to steady-state values. The PIC model (of charged species) and fluid model (for neutral species) are coupled at each time step. The PIC model is electrostatic and electromagnetic standing wave effect30 has been neglected as the chamber dimensions are significantly smaller than the vacuum wavelength at the relevant frequencies (0.8 and 40 MHz). Our PIC model for charged species generally follows the methodology outlined in Refs. 31–34. This PIC model uses the Monte Carlo method to account for collisions. Current at the powered electrode is used in a circuit model to compute voltage drop across the external blocking capacitor. Continuity equation is solved for neutral species, which includes diffusion and production/destruction. This methodology makes it practical to simulate plasmas of molecular gases using this plasma modeling code where neutral radicals can be an important constituent of the gas mixture. For the main gas considered in this article (Ar), one benefit of considering the neutral continuity equation is to take account of the two-step ionization process (Ar → Ar* → Ar+), with Ar* density being self-consistently computed. This two-step process is responsible for 1.7%–3% of electron production in the simulations reported in this article. Solution of neutral continuity equations includes numerical acceleration to speed up evolution to steady-state conditions. The Poisson equation is solved using iterative sparse matrix techniques, utilizing the PETSC library.35 The code has been parallelized using MPI.36 All simulations reported in this article have been done for Ar. Our Ar plasma chemistry mechanism is described in Ref. 26. It includes elastic, metastable excitation, and ionization collisions for Ar; ionization and deexcitation reactions for Ar* metastable; and momentum transfer collisions for Ar+ ions. Both back-scattering and isotropic collisions are considered for Ar+ ions using the cross sections proposed by Phelps.37 Surface processes have been shown to be important for overall plasma dynamics, but their impact is less significant at low pressure.38,39 To focus on the dynamics of bulk plasma electrons and due to the low gas pressure, we have not considered secondary electron emission in the current set of simulations. Electrons are assumed to get fully absorbed at the surfaces with a reflection probability of 0.0. One challenge with 2D PIC simulations in cylindrical geometry is the small differential volume near the axis, which requires a large number of computational particles to adequately resolve the plasma characteristics near r = 0. To keep the total number of particles manageable, we have used nonuniform weight for particles, where weight is defined as the actual number of electrons or ions per PIC macroparticle. Initial particle weight (wi) is proportional to W, h i2 r W(r) ¼ (1 α) þ α , R (1) where R is the maximum radius in the geometry, α is a constant, and r is the radial location of the particle. α = 0.05 for the 2D simulations reported in this article. As particles move to smaller radii during the simulation and wi/W(r) exceeds 2, the particles are split 40, 032202-2 ARTICLE into two particles with ½ the weight but otherwise identical particle characteristics. The smaller weight particles can move to larger radii as well, and particle merging is important to avoid unrestricted growth in the number of particles. We describe our particle merging algorithm in the Appendix. Some kinetic information is always lost when particles are merged. To avoid energy distribution distortion induced by particle merging, particles are merged sparingly: once per 50 000 time steps in the simulations reported. A slightly nonuniform mesh is used for the simulations reported in this article with dx and dz of approximately 1 mm. In the absence of energetic secondary electrons, we have used dt = 50 ps, which satisfies the Courant condition for the electrons in the plasma. The time-averaged modeling results presented in this article have been averaged over the last 800 kHz cycle (=50 cycles of 40 MHz) of the simulation. III. MODELING RESULTS avs.scitation.org/journal/jvb for sinusoidal and rectangular LF voltages in Fig 2(b) for the cases VLF = 900 V; V40 = 250 V for the sinusoidal LF voltage simulation and V40 = 400 V for the rectangular LF wave. These voltages have been plotted for the final 1.25 μs of the simulation when plasma and electrical properties have reached periodic steady-state. As the chamber is electrically asymmetric, a DC bias also builds up at the capacitor, which appears at the electrode. In addition, as the mean voltage of the rectangular wave in Fig. 2(a) is not zero, the DC component of the rectangular wave is also blocked by the capacitor. All simulations reported in this article have been done for 250 μs (10 000 cycles of 40 MHz, 200 cycles of the LF waveform) for VLF in the range of 500–900 V. V40 = 250 V for sinusoidal LF bias and V40 = 400 V for rectangular wave LF bias for reasons explained later in this article. The plasma and electrical characteristics are observed to reach periodic steady-state in 250 μs for all conditions. To illustrate convergence of the simulations, we have plotted spatially averaged electron density (ne), Ar* density (nAr*), and voltage across the blocking capacitor (VC) in Fig. 3. The results The two-dimensional (2D) simulations in this article have been done for the plasma reactor shown in Fig. 1. A combination of fHF = 40 MHz and low frequency (fLF = 800 kHz) bias voltage Vs(t) = V40 sin(2πfHFt) + VLFGLF(t) is applied to the bottom electrode. The top electrode and the chamber sidewalls are grounded. A blocking capacitor C = 2 nF is also connected to the bottom electrode. The two electrodes have a radius of 8 cm and are separated by 2.5 cm. All simulations have been done for Ar plasma at 20 mTorr. The simulations have been done using the sinusoidal and rectangular LF voltage waveforms GLF(t) shown in Fig. 2(a). The duty cycle of the rectangular wave (fraction of time at the most negative voltage) is 80%, and the voltage rise and fall times are 50 ns. The voltage magnitude is scaled to the level specified for individual simulations. The combined voltage at the powered electrode is shown FIG. 1. Schematic of the capacitively coupled plasma reactor used for simulations in this article. J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS FIG. 2. (a) Low frequency 800 kHz voltage waveforms used in the simulations. These waveforms are scaled to the voltages specified in individual simulations. (b) Voltage at the powered electrode during the final 800 kHz time period of the simulation. These waveforms correspond to 400 V 40 MHz + 900 V rectangular wave and 250 V 40 MHz + 900 V sinusoidal wave simulations. Simulations have been done for Ar plasma at 20 mTorr. 40, 032202-3 ARTICLE avs.scitation.org/journal/jvb FIG. 3. Spatially averaged electron density (ne), density of Ar* (nAr*), and voltage on the capacitor (VC) for (a) 400 V 40 MHz + rectangular 700 V LF bias and (b) 250 V 40 MHz + 700 V sinusoidal LF voltage. These simulations have been done for Ar plasma at 20 mTorr. in Fig. 3(a) are for 400 V 40 MHz + rectangular 700 V voltage, and Fig. 3(b) results are for 250 V 40 MHz + 700 V sinusoidal LF voltage. VC is negative for the sinusoidal LF bias due to the smaller size of the powered electrode compared to the grounded surfaces. VC is negative but smaller for the rectangular LF bias as the DC component of the bias waveform drops across the blocking capacitor as well. One of the main reasons for modifying the LF voltage waveform is to control the IEDF. We have shown the IEDF at both the powered and grounded electrodes for rectangular wave LF bias in Fig. 4 and for sinusoidal wave LF voltage in Fig. 5. Results are shown for VLF = 500, 700, and 900 V. The IEDFs computed by our PIC model have been previously validated against experimental measurements,40 albeit at lower voltages. The IEDF at the powered electrode has a sharp peak with rectangular wave LF bias [Fig. 4(a)], and the location of this peak shifts to higher energy with increasing bias voltage VLF. There is also significant population of low energy ions, which are produced during the positive voltage phase of the LF waveform and through collisions in the thick sheath during the negative LF voltage phase. For similar LF voltages, the IEDF is wider with sinusoidal bias voltage [Fig. 5(a)] and the low energy population is also higher than the rectangular wave. These changes can be attributed to the constantly evolving nature of the powered electrode sheath voltage, which results in a bimodal IEDF at low frequencies. With a thick sheath, ion-neutral collisions are, however, making the low energy peak broader. The J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS FIG. 4. IEDF at the (a) powered electrode and (b) grounded electrode. These results are for Ar plasma at 20 mTorr and 400 V 40 MHz. The 800 kHz LF voltage is rectangular with an amplitude of 500, 700, or 900 V. IEDF at the opposite grounded electrode is wider with rectangular LF bias [Fig. 4(b)] compared to sinusoidal bias [Fig. 5(b)]. The high energy ions for rectangular wave bias bombard the grounded electrode during the positive phase of the rectangular wave while the low energy ions leave the plasma when the powered electrode LF voltage is negative. We next discuss the 2D simulation results. Results are first presented for both the rectangular and sinusoidal wave LF bias, which is followed by a detailed physics discussion. The timeaveraged potential Φave is shown in Fig. 6 for a range of voltages for the rectangular wave LF bias. These results are for V40 = 400 V and 20 mTorr in Ar. The DC voltage at the powered electrode is mentioned in the figure, and it increases in magnitude with increasing VLF. The potential in the plasma bulk is reasonably uniform. The radial gradient in the potential, especially for the highest VLF simulations, results in a radial electric field. This radial field is a consequence of the reactor geometry and plasma uniformity, but, in turn, influences plasma uniformity through ambipolar diffusion. The sheath at the powered electrode gets thicker with increasing VLF. Corresponding time-averaged electron density ne is 40, 032202-4 ARTICLE avs.scitation.org/journal/jvb FIG. 5. IEDF at the (a) powered electrode and (b) grounded electrode. These results are for Ar plasma at 20 mTorr and 250 V 40 MHz. The 800 kHz LF voltage is sinusoidal with an amplitude of 500, 700, or 900 V. shown in Fig. 7. The electron (and Ar+) density decreases with increasing VLF, which is consistent with previous data in the literature.18 Density reduction is due to plasma production in a smaller region at larger VLF and enhanced plasma loss at the powered electrode. Spatially, the plasma density peaks at the chamber center when VLF = 500 V. As VLF is increased, the plasma spreads out in the radial direction, but the charged species densities become uniform only for a narrow range of VLF. With increasing VLF, the plasma splits into two regions, and ne peaks at both the chamber center and near the electrode edge. The source for the production of electrons is shown in Fig. 8. The spatial distribution of the source is generally like the electron density profile, except that we can observe plasma production in the time-averaged sheath region as well. Production in this region mainly occurs when the LF voltage is positive and the sheath collapses in front of the powered electrode. During this time, plasma is efficiently produced through stochastic heating by the 40 MHz source adjacent to the powered electrode. The time-averaged potential for sinusoidal LF waveform is shown in Fig. 9 for a range of bias voltages. These results are for J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS FIG. 6. Time-averaged plasma potential for 800 kHz rectangular wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 400 V 40 MHz. 40, 032202-5 ARTICLE FIG. 7. Time-averaged electron density for 800 kHz rectangular wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 400 V 40 MHz. J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS avs.scitation.org/journal/jvb 250 V at 40 MHz and 20 mTorr in Ar. A lower 40 MHz voltage has been used for sinusoidal wave to attempt to get approximately similar ne with the two bias waveforms. We discuss later why 40 MHz couples more efficiently with sinusoidal wave bias, thus requiring a smaller 40 MHz voltage to obtain similar ne. The potential in the plasma bulk is reasonably uniform, and the DC voltage at the powered electrode increases in magnitude with increasing VLF. The sheath at the powered electrode gets thicker with increasing VLF. Comparing the results in Figs. 6 and 9, one can observe that the “time-averaged” sheath is thicker with rectangular wave LF bias than with sinusoidal waveform, which is primarily because the sheath is fully expanded for a longer period with rectangular wave. Corresponding time-averaged ne is shown in Fig. 10. The electron density peaks at the chamber center when VLF = 500 V. As VLF is increased, ne decreases and the sheath gets thicker, which is observed with rectangular wave bias as well. However, the plasma peak remains at the chamber center until larger VLF with sinusoidal LF bias. The plasma expands in the radial direction becoming more uniform at higher VLF. The time-averaged source of electron and Ar+ ion production is shown in Fig. 11. The plasma is produced reasonably uniformly between the two electrodes for the range of VLF considered in this article. Compared to the results in Fig. 8, one can observe that sources are smaller with sinusoidal wave bias for comparable plasma densities, which is primarily due to the lower 40 MHz voltage. Some of the salient differences between the two LF bias waveforms are that (1) a larger 40 MHz voltage is used with rectangular wave for comparable ne and (2) ne profile evolves differently at higher LF voltages. We next present detailed modeling results to explain these trends. When we reach steady-state, plasma production and loss balance each other. In an Ar plasma, charged species are primarily lost at the surfaces. We have shown time-averaged ion flux to the powered electrode for the two LF bias waveforms in Fig. 12. The ion flux does not change significantly with LF voltage even though the electron and Ar+ densities decrease by a factor of 2 between VLF = 500 and 900 V. This relative insensitivity is because the ion drift current increases with an electric field. The effect of an electric field on ion flux is particularly noticeable at the edge of the powered electrode where the electric field is larger due to the adjacent grounded wall. Ion flux is larger at the electrode edge than at the chamber center even though charged species densities are comparable or lower near the electrode edge. Between the two LF bias waveforms, the ion flux is noticeably higher for rectangular wave than for sinusoidal wave. This difference in ion flux is because the voltage at the powered electrode remains at the peak negative value for a longer period for rectangular LF voltage so ions get extracted more strongly. On a time-averaged basis, an equal number of electron and Ar+ leave the plasma in steady-state so electron loss is higher with rectangular wave too. Due to higher plasma loss with rectangular wave than sinusoidal LF bias, a larger 40 MHz voltage is needed with rectangular LF bias to obtain plasma of comparable density. The plasma is not produced similarly throughout the LF cycle. As explained below, the time variation of plasma production strongly influences the plasma profile. We have shown a spatially integrated source of electrons versus time during the last four LF cycles in Figs. 13(a) and 14(a) for rectangular and sinusoidal LF 40, 032202-6 ARTICLE FIG. 8. Time-averaged electron source for 800 kHz rectangular wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 400 V 40 MHz. J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS avs.scitation.org/journal/jvb FIG. 9. Time-averaged plasma potential for 800 kHz sinusoidal wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 250 V 40 MHz. 40, 032202-7 ARTICLE FIG. 10. Time-averaged electron density for 800 kHz sinusoidal wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 250 V 40 MHz. J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS avs.scitation.org/journal/jvb FIG. 11. Time-averaged electron source for 800 kHz sinusoidal wave voltage of (a) 500, (b) 600, (c) 700, (d) 800, and (e) 900 V. Other conditions are Ar plasma at 20 mTorr and 250 V 40 MHz. 40, 032202-8 ARTICLE avs.scitation.org/journal/jvb FIG. 12. Ar+ flux at the powered electrode for (a) rectangular wave LF voltage and 400 V 40 MHz and (b) sinusoidal wave LF voltage and 250 V 40 MHz. Simulations have been done for Ar plasma at 20 mTorr. bias waveforms, respectively. These results are for VLF = 900 V. Note that the vertical scales are different in these two graphs. With rectangular LF bias, the plasma is produced more intensely when the low frequency voltage at the powered electrode is positive and the sheath collapses there. During this stage, the sheath can oscillate strongly and stochastic heating due to 40 MHz is more effective. Once the LF voltage at the electrode becomes negative, the sheath expands there and plasma production plummets. With sinusoidal LF voltage, even though plasma production varies during the LF cycle, plasma production occurs over a longer period and the changes are more gradual. This time variation of plasma production in dual-frequency CCPs has been extensively studied,41,42 and it is referred to as frequency coupling in the literature. Plasma production location changes during the LF cycle. We have shown the electron source at different times in Figs. 13(b)–13(d) and 14(b) and 14(c) for rectangular and sinusoidal LF waveforms, respectively. Average of the source in discrete time windows is plotted to reduce the statistical noise and more easily explains the trends using static images. Note that different J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS FIG. 13. (a) Spatially averaged electron source during the final four low frequency cycles of the simulation. Time-averaged electron source for (b) 0.0–0.1 fraction of the LF cycle (c) 0.1–0.2 fraction of the LF cycle and (d) 0.3–0.9 fraction of the LF cycle. These results are for Ar plasma at 20 mTorr generated using 400 V at 40 MHz and 900 V at 800 kHz rectangular wave. 40, 032202-9 ARTICLE avs.scitation.org/journal/jvb FIG. 14. (a) Spatially averaged electron source during the final four low frequency cycles of the simulation. Time-averaged electron source for (b) 0.1–0.3 fraction of the LF cycle and (c) 0.3–0.9 fraction of the LF cycle. These results are for Ar plasma at 20 mTorr generated using 250 V at 40 MHz and 900 V at 800 kHz sinusoidal wave. scales have been used for the different time fraction ranges. During the sheath collapse phase with rectangular LF wave, plasma production occurs in the whole interelectrode region with slightly higher production at the chamber center. Plasma production profile during this time mimics the plasma density profile. This intense production, however, occurs for the short time. As the LF voltage at the powered electrode becomes negative, the sheath expands at the powered electrode, making it difficult for plasma to diffuse between the chamber center and edge. For a large fraction of the J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS FIG. 15. (a) Radial flux, (b) vertical flux, and (c) energy of electrons at 0.0412 fraction of the low frequency 800 kHz cycle. Vectors representing the electron flux are also superimposed on the flux plots. These results are for Ar plasma at 20 mTorr excited by 400 V at 40 MHz and 900 V at 800 kHz rectangular wave. LF cycle, the plasma is produced at a slow rate and production strongly occurs beyond the electrode edge where the sheath is thin. This plasma is not able to diffuse to the chamber center due to the thin plasma region, effectively splitting the plasma into two regions. With sinusoidal LF wave, plasma production does vary 40, 032202-10 ARTICLE between the sheath collapse and expansion phases. However, the sheath fully expands for only a short period, so production occurs more uniformly during both these phases. In Fig. 13(a), we can observe a spike in plasma production at the beginning of the positive voltage phase for rectangular voltage waveform. Although only a few percent of the plasma is produced during this period, the electrons in the sheath have been shown to have significant energy then.18,20 It is, therefore, useful to examine the electrons during this phase from the uniformity perspective. We have shown the electron flux in the plasma and the electron energy just after the sheath has collapsed in Fig. 15. On a timeaveraged basis, an equal number of electrons and ions leave the plasma at the surfaces during steady-state. However, with rectangular LF wave, ions exit from the plasma for a long fraction of the LF cycle. For the short period when the sheath collapses, the electrons are compelled to rush out and the powered electrode is bombarded by energetic electrons. Electric field has been shown to reverse for a short time to assist with the production of the large electron flux.18,20 These energetic electrons have sufficient energy to ionize and excite with electron energy higher near the electrode edge due to a higher electric field there. However, due to the low gas pressure, most of these energetic electrons exit at the electrode. We can notice that the electron flux is higher and electrons are more energetic near the electrode edge. Both the electron flux and energy are higher at the electrode edge due to a higher electric field in that region. IV. CONCLUSIONS 2D PIC modeling has been used to examine the effect of LF voltage waveform on plasma characteristics in a dual-frequency (40 + 0.8 MHz) CCP. In such a plasma with disparate frequencies, the low frequency voltage usually has a strong influence on the IEDF but contributes less to plasma generation. Past studies have also shown that the LF voltage waveform can be used to control the IEDF. In particular, a rectangular voltage waveform with a small positive period is known to yield a narrow nearly monoenergetic IEDF. This paper focuses on the effect of the LF voltage waveform on plasma uniformity. A two-dimensional PIC model is used for this investigation to adequately treat electron kinetic effects at low pressure, especially during sharp transitions for the rectangular LF waveform. The effect of LF voltage amplitude on plasma uniformity is compared for sinusoidal and rectangular waveforms. When the LF voltage is low, the charged species densities peak at the chamber center at the low pressure considered (20 mTorr). This centerpeaked density profile is due to ample diffusion at low pressure and higher losses at the chamber periphery. As the LF voltage is increased, the sheath gets thicker at the powered electrode and charged species densities decrease for a constant 40 MHz voltage. The plasma profile, however, evolves differently depending on the LF voltage waveform. With sinusoidal LF voltage, the plasma spreads out between the electrodes as the LF voltage is increased. However, the plasma splits into two regions with rectangular LF voltage waveform: a peak in ne at the chamber center and another peak near the electrode edge. This double-peaked density profile with rectangular wave can be attributed to the time (during the LF cycle) and location where the plasma is generated. Stochastic J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS avs.scitation.org/journal/jvb heating due to 40 MHz is the main source of plasma production under the conditions considered. 40 MHz produces plasma most efficiently when the rectangular wave is positive and the sheath is thin at the powered electrode. Plasma production during this phase occurs mostly uniformly between the electrodes, but this period of uniform plasma production is short. When the LF voltage becomes negative, the sheath expands over the electrodes and the sheath is only thin near the electrode edge. Furthermore, the electric field is larger near the electrode edge due to the adjacent grounded wall. Plasma is produced near the electrode edge during the longer negative voltage phase of the rectangular LF voltage, resulting in a double-peaked plasma density profile. Many different designs for capacitively coupled plasma reactors are used in practice. Although the principles governing plasma generation and transport discussed in this article are expected to be generally applicable, the reported results are specific to the reactor geometry considered. Overall plasma uniformity can, for example, be optimized by modifying the chamber design at the electrode edges and by changing the volume beyond the electrodes. AUTHOR DECLARATIONS Conflict of Interest The authors have no conflicts to disclose. DATA AVAILABILITY The data that support the findings of this study are available from the corresponding author upon reasonable request. APPENDIX: PARTICLE MERGING Particle merging is used in our PIC plasma model to limit unrestricted growth in the total number of PIC particles due to particle splitting. In the particle merging scheme, four particles (Nos. 1–4) of the same type in the same plasma cell are merged into two particles (a, b) using the following methodology: 1. Referring to Fig. 16, particles are only merged in cells that are surrounded by “plasma nodes.” In these cells, we subdivide particles of each type into eight groups based on the direction of their velocity (+/−vx, +/−vy, +/−vz). Candidate particles for merging are chosen from the same velocity group. 2. The merged particles need to satisfy the following conservation equations: ωx ¼ ωa þ ωb ¼ X4 ωx v x ¼ ωa v a þ ωb v b ¼ ωx εx ¼ ωa kv a k2 þ ωb kv b k2 ¼ ii¼1 ωi , X4 ωi v i , (A2) ωi kv i k2 , (A3) ii¼1 X4 ii¼1 (A1) 40, 032202-11 ARTICLE avs.scitation.org/journal/jvb ωa α ωb β ¼ 0, (A9) ωx ðϵx kv x k2 Þ ¼ ωa α2 þ ωb β 2 , (A10) ωx kqx k ¼ ωa α3 ωb β 3 : (A11) E2 ¼ ϵx kv x k2 , (A12) If we define θ¼ α , E (A13) Eqs. (A8)–(A11) can be combined to obtain θ2 1 θkqx k ¼ 0: E3 (A14) Equation (A14) can be solved to determine θ, which can then be used in Eqs. (A5)–(A13) to obtain ωa, ωb, va, and vb. FIG. 16. Definitions used for describing the particle merging algorithm. nij are the densities at the adjacent plasma nodes, and x and z are normalized in the range [0,1]. ωx qx ¼ ωa (va v x )kva v x k2 þ ωb (v b vx )kv b v x k2 X4 ¼ ω (v v x )kv i vx k2 , (A4) ii¼1 i i where some simplifications have been made as all particles have identical mass. For a vector A, we have defined kAk2 ¼ A A: Following the methodology proposed in Ref. 43, we define new variables α, β, and e, where v a ¼ vx þ αe, (A5) v b ¼ v x βe, (A6) q e¼ x : kqx k J. Vac. Sci. Technol. B 40(3) May/Jun 2022; doi: 10.1116/6.0001732 Published under an exclusive license by the AVS ωa (1 xa )(1 za ) þ ωb (1 xb )(1 zb ) ¼ n11 , (A15) ωa xa (1 za ) þ ωb xb (1 zb ) ¼ n12 , (A16) ωa (1 xa )za þ ωb (1 xb )zb ¼ n21 , (A17) ωa xa za þ ωb xb zb ¼ n22 : (A18) Combining these equations, we obtain xb ¼ n12 þ n22 ωa xa , ωb ωb (A19) zb ¼ n21 þ n22 ωa za : ωb ωb (A20) (A7) Inserting Eqs. (A5)–(A7) into Eqs. (A1)–(A4), we obtain the following equations that need to be solved for ωa, ωb, α, and β: ωx ¼ ωa þ ωb , (3) Knowing the velocities and weights of the merged particles, the next goal is to determine their locations. To find the merged particle locations in 2D, we enforce the condition that the species density at plasma nodes does not change due to merging. Therefore, knowing the density at the surrounding plasma nodes (n11, n12, n21, n22) in Fig. 16, the merged particle locations (xa, za) and (xb, zb) need to satisfy the following constraints, where the positions are defined in a normalized cell with dimensions (1,1): (A8) The values of xa, xb, za, and zb need to be in the range [0,1]. However, for given densities at the nodes, ωa, and ωb, Eqs. (A19) and (A20) can be used to ascertain that the valid ranges for xa and za are even more restricted. 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