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Elementary gas‐phase reactions of radical species during chemical vapor deposition of silicon carbide using CH 3 SiCl 3
Author(s) -
Sato Noboru,
Funato Yuichi,
Shima Kohei,
Sugiura Hidetoshi,
Fukushima Yasuyuki,
Momose Takeshi,
Koshi Mitsuo,
Shimogaki Yukihiro
Publication year - 2021
Publication title -
international journal of chemical kinetics
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.341
H-Index - 68
eISSN - 1097-4601
pISSN - 0538-8066
DOI - 10.1002/kin.21470
Subject(s) - chemistry , chemical vapor deposition , radical , isomerization , decomposition , silicon carbide , silicon , chemical vapor infiltration , kinetic energy , yield (engineering) , analytical chemistry (journal) , thermodynamics , organic chemistry , catalysis , physics , quantum mechanics , ceramic
We established a kinetic model (the UT2017 model) for chemical vapor deposition of silicon carbide (SiC) from methyltrichlorosilane (CH 3 SiCl 3 , MTS)/H 2 , and quantitatively identified CH 2 SiCl 3 as one of the SiC film‐forming species. In a previous study, we established a kinetic model (the UT2014 model), which reproduced the overall decomposition of MTS, but had not validated it in terms of radicals. In the present study, we first validated the UT2014 model by comparing it with the experimental results of radical production from MTS by Lemieux et al, without H 2 present. The UT2014 model did not reproduce the production of CH 2 Cl from MTS at 1247°C. We found that the reactions of CH 2 SiCl 3 isomerization to CH 2 ClSiCl 2 and CH 2 ClSiCl 2 decomposition to CH 2 Cl and SiCl 2 were important for the production of CH 2 Cl from MTS. We re‐calculated those constants in pressure‐dependent formulas using the Rice‐Ramsperger‐Kassel‐Marcus method at the CBS‐QB3 level. These chemistries were added to the UT2014 model to yield the UT2017 model, which reproduced the production of radicals, including CH 2 Cl. Finally, using the UT2017 model, we simulated the gas composition under typical SiC chemical vapor infiltration conditions, which comprised mainly MTS and H 2 . A comparison of the simulation results with the partial pressure of film‐forming species in our previous report suggested that CH 2 SiCl 3 was the possible film‐forming species of SiC from MTS/H 2 . For quantitative verification, we estimated the distribution of the partial pressure of CH 2 SiCl 3 in our reactor while considering the consumption of CH 2 SiCl 3 on the SiC surface. The values from this simulation result were almost identical to our experimental results for all positions in the reactor. Thus, we showed quantitatively that CH 2 SiCl 3 is the film‐forming species of SiC.