We established a gas‐phase, elementary reaction model for chemical vapor deposition of silicon carbide from methyltrichlorosilane (MTS) and H₂, based on the model developed at Iowa State University (ISU). The ISU model did not reproduce our experimental results, decomposition behavior of MTS in the gas phase in an environment with H₂. Therefore, we made several modifications to the ISU model. Of the reactions included in existing models, 236 were lacking in the ISU model, and thus were added to the model. In addition, we modified the rate constants of the unimolecular reactions and the recombination reactions, which were treated as a high‐pressure limit in the ISU model, into pressure‐dependent rate expressions based on the previous reports (to yield the ISU+ model), for example, H₂(+M) → H + H(+M), but decomposition behavior remained poorly reproducible. To incorporate the pressure dependencies of unimolecular decomposition rate constants, and to increase the accuracies of these constants, we recalculated the rate constants of five unimolecular decomposition reactions of MTS using the Rice‐Ramsperger‐Kassel‐Marcus method at the CBS‐QB3 level. These chemistries were added to the ISU+ model to yield the UT2014 model. The UT2014 model reproduced overall MTS decomposition. From the results of our model, we confirmed that MTS mainly decomposes into CH₃ and SiCl₃ at the temperature around 1000°C as reported in the several studies.

中文翻译：

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CH3SiCl3 / H2碳化硅化学气相沉积过程中基本气相反应的建模

基于爱荷华州立大学（ISU）开发的模型，我们建立了从甲基三氯硅烷（MTS）和H _2进行碳化硅化学气相沉积的气相基本反应模型。ISU模型没有重现我们的实验结果，即MTS在H ₂环境下在气相中的分解行为。因此，我们对ISU模型进行了一些修改。现有模型中包含的反应中，ISU模型中缺少236种，因此已添加到模型中。此外，我们根据以前的报告将单分子反应和重组反应的速率常数（在ISU模型中被视为高压极限）修改为压力依赖性速率表达式（以生成ISU +模型），例如H₂（+ M）→H + H（+ M），但分解行为仍然难以再现。为了合并单分子分解速率常数的压力依赖性，并增加这些常数的准确性，我们使用Rice-Ramsperger-Kassel-Marcus方法在CBS-QB3水平上重新计算了MTS的五个单分子分解反应的速率常数。这些化学成分已添加到ISU +模型中，以生成UT2014模型。UT2014模型重现了MTS的整体分解。从我们的模型结果中，我们证实了MTS主要分解为CH ₃和SiCl ₃，如几项研究报道。