Electron bounce resonance heating in dual-frequency capacitively coupled oxygen discharges Yong-Xin Liu1, Quan-Zhi Zhang1, Jia Liu1, Yuan-Hong Song1, Annemie Bogaerts2, and You-Nian Wang1,a) 1 School of Physics and Optoelectronic Technology, Dalian University of Technology, Dalian 116024, China 2 Department of Chemistry, University of Antwerp, Campus Drie Eiken, Universiteitsplein 1, BE-2610 Wilrijk-Antwerp, Belgium Absract: The BRH in DF CCPs operated in oxygen has been studied by different experimental methods and a particle-in-cell/Monte Carlo collision (PIC/MCC) simulation, and compared with the electropositive argon discharge. All these experimental observations are explained by PIC/MCC simulations, which show that in the oxygen discharge the bulk electric field becomes quite strong and is out of phase with the sheath field. Keywords: Dual-frequency, electron density, hairpin probe, oxygen discharge a) E-mail: [email protected] 1. Introduction 2. Experiment setup and simulation Recently, the bounce resonance heating (BRH) effect has been experimentally observed in in (2/60 MHz) capacitive discharge chamber [9]. When electropositive argon, and it was found to markedly conducting the optical measurements, the O2 discharge is enhance the discharge performance under certain diluted with 5% Ar, as it is difficult to probe the emission conditions. applications, from the direct excitation of molecule O2. The measured electronegative gases are most frequently employed. electron density by the hairpin probe is corrected by They are different from electropositive gas discharges in using the fluid model described by Piejak [10]. In the some basic, important features, such as the development experiment, we will compare the different behavior of of double layers [1, 2], a strong electric field and thus a BRH in Ar and O2 and study the effect of high-frequency high ionization rate in the bulk [3], more pronounced (HF) power on the BRH in the O2 discharge. However, in real DF CCPs Our experiments are performed in a parallel-plate DF modulation of the bulk electric field [4, 5], and a discharge mode transition induced by voltage or pressure[6-8]. These pronounced differences will have a substantial impact on the BRH, and the resultant electron energy probability function (EEPF) determines the basic discharge dynamics, such as dissociation, excitation, and ionization in electronegative discharges. Therefore, it is of fundamental importance to study the features of BRH in electronegative discharges. Fig. 1 Schematic diagrams of the dual-frequency capacitively coupled plasma reactor. Our simulations, which serve as a numerical explanation of the experiments of O2 and Ar discharges, are based on the standard one-dimensional in space the Ar discharge, the most significant BRH effect in the three-dimensional in velocity (1D3V) electrostatic PIC O2 discharge occurs at a somewhat larger gap, with the MCC method. More details can be found in Ref. [9]. To resonant peak broadened. The larger resonance gap and shed light on the BRH behavior at different HF powers in broader peak in the O2 discharge is related to the the experiments of O2, we compare the spatiotemporal electronegative discharge structure. In simulations, we distribution of various plasma quantities (i.e., the observed a narrower bulk region and higher bulk electric electron impact ionization rate, bulk electric field, field. Note that the position of the resonance peak is trajectory of a typical bouncing electron and its energy) almost independent of the pressure in both Ar [9] and O2. for a range of HF voltages. In the case of the O2 (ii) At L > 2:5 cm, the positive ion and electron densities discharge, the charged particles O2+, O, and the drop monotonously in the O2 discharge upon increasing electrons are traced using cross sections from Ref. 23. L, while the plasma density rises in the Ar case. This is For Ar, the cross sections are the same as in Ref. [9]. due to the more significant drop of the BRH with increasing L in the O2 discharge. It is worth to mention that our PIC MCC simulations have qualitatively 3. Results and discussion reproduced the experimental density curves both in Ar and O2. 3.1 electrode gap effect 3.2 HF power effect 0.4 0.8 - e density in argon e density in oxygen by hairpin resonant probe 1 2 3 4 5 0.2 -3 cm ) + 1.2 O2 density (a.u.) 0.6 0.4 2.8 80 W 60 W 40 W 20 W 10 0.8 Electron density (10 -3 1.6 Ion density (10 2.0 10 cm /a.u.) + Ar density in argon + relative O2 density in oxygen by floating double probe 2.4 2.4 2.0 1.6 6 Gap length (cm) Fig. 2 Experimental measurements: positive ion and electron density versus gap length, in Ar (black) and O2 1.2 1 2 3 4 5 6 Gap length (cm) (red lines) discharges, at a fixed HF and LF power of Fig. 3 Experimental measurements in the O2 plasma: 30W and 100 W, respectively. Note that the pressure relative O2+ Ion density at the discharge center versus L, increases from 1.3 Pa in Ar to 4.0 Pa to sustain the O2 at a range of HF powers PH for a fixed LF power PL of discharge. 100 W, at a gas pressure of 4.0 Pa. Fig. 2 illustrates the measured positive ion density and The effect of HF power PH on the BRH in the O2 electron density versus gap length L, at a fixed HF and discharge is shown in Fig. 3, which displays the low-frequency (LF) power of 30W and 100 W, for the Ar measured relative O2+ ion density versus L at different and O2 discharge (black and red curves, respectively). values of PH with a fixed PL of 100W and a pressure of The Ar+ ion density is measured in absolute terms, 4.0 Pa. At lower PH, both the O2+ ion density peak whereas the O2+ density is only obtained in relative gradually drops and almost disappears at PH = 20 W, terms. The BRH effect is illustrated by the peak in ion which indicates a suppressed BRH. It should be noted and electron density at a certain gap length, called the that the results are quite different from the electropositive resonant gap length. From this figure, the differences of Ar discharge, where the BRH is hardly affected by PH the BRH effect between Ar and O2 discharges can be [9]. This is attributed to the fact that the O2 discharge generally summarized as followings. (i) Compared with experiences a mode transition from electropositive to electronegative due to the lower amount of sheath explained because at relatively low driving frequency the heating with the drop of PH. This mode transition electrons can respond to the rf electric field whereas they induced by the driving voltage has been observed in gradually fail to follow the rf field at higher frequencies, CCPs with other electronegative gases as well [6, 7]. i.e. at the driving frequency f > 60 MHz. Note that this 3.3 Gas pressure phase relationship between the plasma bulk field and the Fig. 4 illustrates the measured positive-ion O2+ density sheath field at different driving frequencies is consistent versus electrode gap L at different pressures. At higher with the results in [13]. pressures, the maximum around the resonance gap 0.500 diminishes gradually and almost disappears at 12 Pa, electronegative discharges, two different pressure effects are responsible for the BRH. First, as the electron mean free path is inversely proportional to the pressure, the resonance electrons simply cannot bounce long time enough at high pressures, to gain sufficient energy before being stopped or re-directed by a collision. This effect also occurs in a pure argon discharge [12]. Moreover, an additional pressure effect occurs in the oxygen discharge, namely the enhanced bulk electric field reversal, which 4.0 Pa 6.0 Pa 8.0 Pa 12.0 Pa + O2 density (a.u.) 2.2 2.0 1.8 0.375 0.250 0.125 0.000 0 20 40 60 80 100 120 Driving frequency (MHz) Fig. 5 Phase delay of the plasma bulk field with respect to the sheath field, θ, as a function of the driving suppresses the BRH at higher pressures. 2.4 Phase delay / which indicates again a suppression of the BRH. In frequency. 4. Conclusion 1.6 1.4 We investigated the electron bounce resonance heating 1.2 (BRH) in dual-frequency capacitively coupled plasmas 1.0 operating in oxygen by different experimental methods 0.8 1 2 3 4 5 6 Electrode gap (cm) and a particlein-cell/Monte Carlo collision (PIC/MCC) simulation, and compared with the electropositive argon Fig. 4 Measured positive-ion (O2+ ) density versus discharge. In comparison with the electropositive argon electrode gap L in the oxygen discharge at different discharge, the BRH in the electronegative oxygen pressures with a fixed HF and LF power of 30W and discharge tends to happen at larger electrode gaps. This 100W is related to the peculiar oxygen discharge structure, i.e. 3.4 HF frequency effect the development of a double layer in the sheath and the Fig. 5 illustrates the phase delay of the plasma bulk narrower bulk region and higher reversal electric field in field with respect to the sheath field, as a function of the the bulk. At electrode gap L > 2.5 cm, the positive-ion driving frequency. At the driving frequency of 13.56 (and electron) density drops monotonically in the oxygen MHz, the bulk electric field is in phase with the sheath, discharge upon increasing electrode gap, whereas it rises so θ is zero. With the increase in the driving frequency, (after an initial drop) in the argon case. This indicates the phase of the bulk electric field will delay with respect that the BRH drops significantly at electrode gaps larger to the sheath field, the phase delay θ increases rapidly than the resonance length, in the oxygen discharge. and tends to reach its maximum π/2 when the driving PIC/MCC simulation results show that in the oxygen frequency approaches 120 MHz. This behavior can be discharge, the bulk electric field reversal becomes quite strong and is out of phase with the sheath field. Therefore, it retards the resonance electrons when Reference traversing the bulk, resulting in a suppressed BRH. [1] N. Nakano, N. Shimura, Z.-L. Petrovic´, and T. Finally, in addition to the effect of the discharge gas Makabe, Phys. Rev. E 49, 4455 (1994). (oxygen versus argon), also the effect of HF power, gas [2] V. A. Lisovskiy and V. D. Yegorenkov, Vacuum 80, pressure and high frequency on the BRH were 458 (2006). investigated, both experimentally and by simulations. It [3] M. Shibata, N. Nakano, and T. Makabe, J. Appl. Phys. appears that the resonance peaks in the positive-ion 77, 6181 (1995). density become weaker with decreasing HF power. This [4] M. Yan, A. Bogaerts, W. J. Goedheer, and R. Gijbels, is attributed to the enhancement of the reversal bulk Plasma Sources Sci. Technol. 9, 583 (2000). electric field when the discharge undergoes a transition [5] M. Yan, A. Bogaerts, and R. Gijbels, J. Appl. Phys. from electropositive to electronegative mode with the 87, 3628 (2000). drop in the HF power. Furthermore, in the pure oxygen [6] J. Schulze, A. Derzsi, K. Dittmann, T. Hemke, J. discharge, the BRH is suppressed with increasing Meichsner, and Z. pressure and it almost diminishes at 12 Pa. This is due to Donko, Phys. Rev. Lett. 107, 275001 (2011). a combined effect of more frequent electron–neutral [7] O. V. Proshina, T. V. Rakhimova, A. T. Rakhimov, collisions and enhanced bulk electric field reversal at and D. G. Voloshin, high pressures. Finally, the BRH was found to depend Plasma Sources Sci. Technol. 19, 065013 (2010). significantly on the high frequency applied, which can be [8] K. Denpoh and K. Nanbu, Jpn. J. Appl. Phys., Part 1 explained based on the phase relation between bulk 39, 2804 (2000). electric field and sheath electric field. [9] Y. X. Liu, Q. Z. Zhang, W. Jiang, W. Q. Lu, and Y. N. Wang, Plasma Sources Sci. Technol. 21, 035010 (2012). [10] R. B. Piejak, V. A. Godyak, R. Garner, B. M. 5. Acknowledgement Alexandrovich, and N. Sternberg, J. Appl. Phys. 95, 3785 This work was supported by the Important National (2004). Science and Technology Specific Project (Grant No [11] V. Vahedi and M. Surendra, Comput. Phys. 2011ZX02403-001), Commun. 87, 179 (1995). the National Natural Science Foundation of China (NSFC) (Grand No 11075029), the [12] Liu Y X et al 2012 Plasma Sources Sci. Technol. 21 International Science and Technology Cooperation 035010 Program of China (Grant No 2012DFG02150) and the [13] Yan M, Bogaerts A, Gijbels R and Goedheer W J joint research project in the framework of the agreement 2000 J. Appl. Phys. 87 3628 between MOST and FWO.
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