Kinetic and Microstructure of SiC Deposited from SiCl4-CH4-H2

›› 2009, Vol. 17 ›› Issue (3): 419-426.

Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂

杨艳^1,2, 张伟刚¹

1. State Key Lab of Multi-phase Complex Systems, Ins1. State Key Lab of Multi-phase Complex Systems, Institute of Process Engineering, CAS, Beijing 100190, China;
2. Graduate University of Chinese Academy of Sciences, Beijing 100049, China

收稿日期:2008-07-05 修回日期:2009-04-18 出版日期:2009-06-28 发布日期:2009-06-28
通讯作者: ZHANG Weigang,E-mail:wgzhang@home.ipe.ac.cn
基金资助:
Supported by the One Hundred Talents Program of Chinese Academy of Sciences

Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂

YANG Yan^1,2, ZHANG Weigang¹

1. State Key Lab of Multi-phase Complex Systems, Ins1. State Key Lab of Multi-phase Complex Systems, Institute of Process Engineering, CAS, Beijing 100190, China;
2. Graduate University of Chinese Academy of Sciences, Beijing 100049, China

Received:2008-07-05 Revised:2009-04-18 Online:2009-06-28 Published:2009-06-28
Supported by:
Supported by the One Hundred Talents Program of Chinese Academy of Sciences

摘要/Abstract

摘要： Silicon carbide was prepared from SiCl₄-CH₄-H₂ gaseous precursors by isothermal, isobaric chemical vapor deposition (CVD) at atmospheric pressure and temperatures ranging from 900℃ to 1100℃. Kinetic studies showed that carbosilane of SiH₂Cl₂, SiHCl₃ and SiCl₂ formed from decomposition of SiCl₄ and CH₄ contributed to the deposition of hexangular facet and granular pebble structured SiC. An average apparent activation energy of 152 kJ·mol^-1 was determined. The overall CVD process was controlled not only by the surface reactions but also by complex gas phase reactions. The as-deposited thin film was characterized using scanning electron microscopy, X-ray diffraction and transmission electron microscopy, these analysis showed that the deposited thin film consisted of pure phase of the β-SiC, the growth morphology of β-SiC differs from hexangular facet to granular pebble structures, which varied with substrate length and CVD temperature.

关键词: chemical vapor deposition, SiC, kinetics, microstructure

Abstract: Silicon carbide was prepared from SiCl₄-CH₄-H₂ gaseous precursors by isothermal, isobaric chemical vapor deposition (CVD) at atmospheric pressure and temperatures ranging from 900℃ to 1100℃. Kinetic studies showed that carbosilane of SiH₂Cl₂, SiHCl₃ and SiCl₂ formed from decomposition of SiCl₄ and CH₄ contributed to the deposition of hexangular facet and granular pebble structured SiC. An average apparent activation energy of 152 kJ·mol^-1 was determined. The overall CVD process was controlled not only by the surface reactions but also by complex gas phase reactions. The as-deposited thin film was characterized using scanning electron microscopy, X-ray diffraction and transmission electron microscopy, these analysis showed that the deposited thin film consisted of pure phase of the β-SiC, the growth morphology of β-SiC differs from hexangular facet to granular pebble structures, which varied with substrate length and CVD temperature.

Key words: chemical vapor deposition, SiC, kinetics, microstructure

杨艳, 张伟刚. Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂[J]. , 2009, 17(3): 419-426.

YANG Yan, ZHANG Weigang. Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂[J]. , 2009, 17(3): 419-426.

参考文献

1 Kim, H.S., Choi, D.J., “Effect of diluent gases on growth behavior and characteristics of chemically vapor deposited silicon carbide films”, J. Am. Ceram. Soc., 82, 331-337(1999).
2 Cagliostro, D.E., Riccitiello, S.R., “Model for the formation of silicon carbide from the pyrolysis of dichlorodimethylsilane in hydrogen(I) Silicon formation from chlorosilane”, J. Am. Ceram. Soc., 76(1), 39-48(1993).
3 Cagliostro, D.E., Riccitiello, S.R., “Model for the formation of silicon carbide from the pyrolysis of dichlorodimethylsilane in hydrogen(II) Silicon carbide formation from silicon and methane”, J. Am. Ceram. Soc., 76(1), 49-53(1993).
4 Cagliostro, D.E., Riccitiello, S.R., “Comparison of the pyrolysis products of dichlorodimethylsilane in the chemical vapor deposition of silicon carbide on silica in hydrogen or argon”, J. Am. Ceram. Soc., 77(10), 2721-2726(1994).
5 Takeuchi, T., Egashira, Y., Osawa, T., Komiyama, H., “A kinetic study of the chemical vapor deposition of silicon carbide from dichlorodimethylsilane precursors”, J. Electrochem. Soc., 145(4), 1277-1284(1998).
6 Papasouliotis, G.D., Sotirchos, S.V., “On the homogeneous chemistry of the thermal decomposition of methyltrichlorosilane:Thermodynamic analysis and kinetic modeling”, J. Electrochem. Soc., 141(6), 1599-1611(1994).
7 Besmann, T.M., Sheldon, B.W., Lowden, R.A., Stinton, D.P., “Vapor-phase fabrication and properties of continuous-filament ceramic composites”, Science, 253, 1104-1109(1991).
8 Sotirchos, S.V., Papasouliotis, G.D., “Experimental study of the atmospheric pressure chemical vapor deposition of silicon carbide from methyltrichlorosilane”, J. Mater. Res., 14, 3397-3409(1999).
9 Loumagne, F., Langlais, F., Naslain, R., “Reactional mechanisms of the chemical vapour deposition of SiC-based ceramics from CH₃SiCl₃/H₂ gas precursor”, J. Cryst. Growth, 155, 205-213(1995).
10 Loumagne, F., Langlais, F., Naslain, R., “Reactional mechanisms of the chemical vapour deposition of SiC-based ceramics from CH₃SiCl₃/H₂ gas precursor”, J. Cryst. Growth, 155, 198-204(1995).
11 Sone, H., Kaneko, T., Miyakawa, N., “In situ measurements and growth kinetics of silicon carbide chemical vapor deposition from methyltrichlorosilane”, J. Cryst. Growth, 219, 245-252(2000).
12 Kaneko, T., Okuno, T., Yumoto, H., “Growth kinetics of silicon carbide CVD”, J. Cryst. Growth, 91(4), 599-604(1988).
13 Lu, Y.M., Leu, I.C., “Microstructural study of residual stress in chemically vapor deposited B-SiC”, Surface Coatings Technol., 124, 262-265(2000).
14 Vorobev, A.N., Karpov, S.Y., Zhmakin, A.I., Lovtsus, Y.N., “Effect of gas-phase nucleation on chemical vapor deposition of silicon carbide”, J. Cryst. Growth, 211, 343-346(2000).
15 Reznik, B., Gerthsen, D., Zhang, W.G., Hüttinger, K.J., “Microstructure of SiC deposited from methyltrichlorosilane”, J. Eur. Ceram. Soc., 23, 1499-1508(2003).
16 Zhang, W.G., Hüttinger, K.J., “CVD of SiC from methyltrichlorosilane. Deposition rates”, Chem. Vap. Depos., 7(4), 167-172(2001).
17 Zhang, W.G., Hüttinger, K.J., “CVD of SiC from methyltrichlorosilane. Composition of the gas phase and the deposit”, Chem. Vap. Depos., 7(4), 173-181(2001)
18 Habuka, H., Watanabe, M., Nishida, M., Sekiguchi, T., “Polycrystalline silicon carbide film deposition using monomethylsilane and hydrogen chloride gases”, Surface Coatings Technol., 201, 8961-8965(2007).
19 Jung, Y.G., Park, S.W., Choi, S.C., “Effect of CH₄ and H₂ on CVD of SiC and TiC possible fabrication of SiC/TiC/C FGM”, Mater. Lett., 30, 339-345(1997).
20 Hu, Z.J., Hüttinger, K.J., “Mechanisms of carbon deposition—A kinetic approach”, Carbon, 40(4), 624-8(2002).
21 Zheng, C.Q., Ran, J.G., New Inorganic Materials, Science Press, Beijing, 87-89(2003).(in Chinese)
22 Zhang, W.G., “Chemical vapor deposition of carbon”, Chemical Vapor Deposition—From Hydrocarbon to Carbon, Science Press, Beijing, 44-51(2007).(in Chinese)
23 Givargizou, E.J., Current Topic in Materials Science, North-Holland, New York, 56(1978).

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Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂

Kinetic and Microstructure of SiC Deposited from SiCl₄-CH₄-H₂

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