プラズマCVDの化学反応工学

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1 CVD Chemical Reaction Engineering of Plasma CVD Tatsuru SHIRAFUJI Key Words: Plasma, Chemical Vapor Deposition, Thin Film, Chemical Reaction Engineering (chemical vapor deposition; CVD) CVD CVD CVD Maxwell CVD CVD CVD 3 CVD 1) (a-si:h) 2 4 CVD vs. PVD (physical vapor deposition; PVD) CVD CVD PVD PVD 10 3 Pa 1 m PVD 100% PVD CVD Dept. Physical Electronics and Informatics, Osaka City University ( Sugimoto, Sumiyoshi-ku, Osaka, Japan)

2 CVD Figure 1 Schematics and features of PVD and CVD. Figure 2 Schematic explanation of the effect of sticking probability on trench coverage profiles. CVD PVD PVD PVD CVD 1 1 CVD PVD PVD CVD PVD PVD CVD CVD vs. CVD CVD CVD CVD CVD CVD CVD CVD CVD 190 nm CVD CVD CVD

3 Figure 3 Schematic illustration of a CCP plasma CVD chamber and elementary processes involved in the plasma CVD process. CVD 5) 6) PET 7, 8) CVD CVD CVD (capacitively coupled plasma; CCP) CVD CVD (ionization) (electron attachment) (excitation) (dissociation) CCP (sheath edge) CVD CVD (d) (a) (b) (b) SiH 4 CVD SiH 4

4 CVD Figure 4 Possible arrangements of atoms (Si). (a) amorphous, (b) hydrogenated amorphous, (c) micro-crystalline and (d) single crystalline. (c) 3 CVD 9,10) (electron energy distribution funciton; EEDF) 11, 12) CVD EEDF Figure 5 Electron impact dissociation cross sections to produce neutral radicals (CF, CF 2 and CF 3) from c-c 4F 8. 9) Please note that the other neutral species can be produced at the same time. SiH 4 H 2 SiH 4 SiH 4 H 2 SiH 4 SiH 4 H 2 SiH 4/H 2 BolSIG + 12) EEDF SiH 4 H 2 10 ev CVD 10 % 90 % EEDF CVD ( Pa) 1 mm 10 μm cm CVD

5 Figure 7 Chemical species in SiH 4 plasma. Figure 6 Selected cross section data sets for SiH 4 and H 2, and EEDF calculated using these cross section data, where E / N is reduced electric field (1 Td = V m 2 ). q m is momentum transport cross section. q i, q a, q d is ionization, attachment and dissociation cross sections, respectively. CVD SiH 4 SiH 3 SiH 2 SiH Si H SiH 3 ( m 3 ) ( nm/s) SiH 4 QMA 13 15) OES 16 18) LIF (Si, SiH) 19 21) IRLAS (SiH 3) 22, 23) ICLAS (SiH 2) 24) 10 SiH 4 SiH 4 + e SiH 3 + H + e 83% (1) SiH 2 + 2H + e 10% (2) 25) SiH 3 83% SiH 2 10 % SiH 3 SiH 2 SiH 3

6 CVD Figure 9 Infrared absorption spectra of the films deposited using HMDSO as a source gas. 6) Figure 8 Effects of branching ratio for the electron impact dissociation of a SiH 4 molecule, where electron density is N e = m -3, dissociation rate coefficient is k d = m 3 s -1. SiH 4 + SiH 2 Si 2H 6 ( ) (3) SiH 4 + H SiH 3 + H 2 ( ) (4) () (m 3 s 1 ) SiH 3 SiH 4 + SiH 3 SiH 3 + SiH 4 (5) SiH 3 SiH 2 SiH 3 1 ms SiH 2 SiH 3 CVD HMDSO ((CH 3) 3SiOSi(CH 3) 3) Si-O-Si Si-CH 3 26) Si-O-Si Si-(CH 3) RF Si-CH 3 SiO (1 β) β

7 a-si:h SiH 3 Si H SiH 3 Figure 10 The two-step sticking process of SiH 3 radicals, which explains a-si:h film deposition process. 27) Figure 11 Sticking-probability dependence of the trench coverage profile. 28) a-si:h SiH 3 SiH 4 27) CVD a-si:h Si-H H H 2 Si Si-Si (b) 28) (β 1) (β 0.1) β = 0 β 0.1 C 5F 8 29) CF x ) 31) (a) (b)

8 CVD Figure 12 Examples of film deposition on reverse-tapered microstructures 29). (a) Shadow zone is not covered with the film. (b) Shadow zone is covered with the film. CVD CVD PVD CVD PVD CVD 1) : (2003). 2) : 68 (1999) ) : 76 (2000) ) A. Matsuda: Jpn. J. Appl. Phys., 43 (2004) ) Y. Wu, H. Sugimura, Y. Inoue, O. Takai: Chem. Vap. Deposition, 8 (2002) ) M. Pagliaro, G. Palmisano, R. Ciriminna: Flexible Solar Cells, Wiley-VCH (2008). 7) : 42 (2005) ) : (2005) ) H. Toyoda, M. Iio, H. Sugai: Jpn. J. Appl. Phys., 36 (1997) ) L. G. Christophorou, J. K. Olthoff: Fundamental electron interactions with plasma processing gases, Kluwer Academic (2004). 11) : (1999). 12) G. J. M. Hagelaar, L. C. Pitchford: Plasma Sources Sci. Technol., 14 (2005) ) B. Drevillon, J. Huc, A. Lloret, J. Perrin, G. de Rosny, J. P. M. Schmitt: Appl. Phys. Lett., 37 (1980) ) Haller: Appl. Phys. Lett., 37 (1980) ) G. Turban, Y. Catherine, B. Grolleau: Thin Solid Films, 67 (1980) ) F. J. Kampas, R. W. Griffith: Solar Cells, 2 (1980) ) T. Hamasaki, H. Kurata, M. Hirose, Y. Osaka: Appl. Phys. Lett., 37 (1980) ) A. Matsuda, K. Nakagawa, K. Tanaka, M. Matsumura, S. Yamasaki, H. Okushi, S. Iizima: Non-Cryst. Solids, (1980) ) P. M. Schmitt, P. Gressier, M. Krishnan, G. de Rosny, J. Perrin: Chem. Phys., 84 (1984) ) Y. Matsumi, T. Hayashi, H. Yoshikawa, S. Komiya: J. Vac. Sci. Technol. A, 4 (1986) ) Tachibana: Mater. Sci. Technology B, 17 (1993) ) C. Yamada, E. Hirota: Phys. Rev. Lett., 56 (1986) ) Itabashi, K. Kato, N. Nishiwaki, T. Goto, C. Yamada, E. Hirota: Jpn. J. Appl. Phys., 27 (1988) L1565-L ) K. Tachibana, T. Shirafuji, Y. Matsui: Jpn. J. Appl. Phys., 31 (1992) ) J. Kushner: J. Appl. Phys., 63 (1988) ) T. Shirafuji, Y. Miyazaki, Y. Nakagami, Y. Hayashi, S. Nishino: Jpn. J. Appl. Phys., 38 (1999) ) A. Matsuda, K. Tanaka: J. Appl. Phys., 60 (1986) ) A. Yuuki, Y. Matui, K. Tachibana: Jpn. J. Appl. Phys., 28 (1989) ) T. Shirafuji, T. Wada, M. Kashiwagi, T. Nakamura, K. Tachibana: Jpn. J. Appl. Phys., 42 (2003) ) E. Capps, N. M. Mackie, E. R. Fisher: J. Appl. Phys., 84 (1998) ) : 75 (1999)

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