We established a kinetic model (the UT2017 model) for chemical vapor deposition of silicon carbide (SiC) from methyltrichlorosilane (CH₃SiCl₃, MTS)/H₂, and quantitatively identified CH₂SiCl₃ 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 H₂ present. The UT2014 model did not reproduce the production of CH₂Cl from MTS at 1247°C. We found that the reactions of CH₂SiCl₃ isomerization to CH₂ClSiCl₂ and CH₂ClSiCl₂ decomposition to CH₂Cl and SiCl₂ were important for the production of CH₂Cl 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 CH₂Cl. Finally, using the UT2017 model, we simulated the gas composition under typical SiC chemical vapor infiltration conditions, which comprised mainly MTS and H₂. A comparison of the simulation results with the partial pressure of film‐forming species in our previous report suggested that CH₂SiCl₃ was the possible film‐forming species of SiC from MTS/H₂. For quantitative verification, we estimated the distribution of the partial pressure of CH₂SiCl₃ in our reactor while considering the consumption of CH₂SiCl₃ 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 CH₂SiCl₃ is the film‐forming species of SiC.

中文翻译：

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使用CH3SiCl3碳化硅化学气相沉积过程中自由基种类的基本气相反应

我们建立了用于从甲基三氯硅烷（CH ₃ SiCl ₃，MTS）/ H ₂进行化学气相沉积碳化硅（SiC）的动力学模型（UT2017模型），并定量确定了CH ₂ SiCl ₃是SiC成膜物质之一。 。在先前的研究中，我们建立了一个动力学模型（UT2014模型），该模型再现了MTS的整体分解，但未在自由基方面进行验证。在本研究中，我们首先通过将其与Lemieux等人在不存在H _2的情况下从MTS自由基产生的实验结果进行比较，来验证UT2014模型。UT2014模型未复制CH ₂的生产在1247°C下来自MTS的Cl。我们发现，CH ₂ SiCl ₃异构化为CH ₂ ClSiCl _2的反应和CH ₂ ClSiCl ₂分解为CH ₂ Cl和SiCl ₂的反应对于由MTS生产CH ₂ Cl至关重要。我们在CBS-QB3级别使用Rice-Ramsperger-Kassel-Marcus方法重新计算了压力相关公式中的那些常数。这些化学成分已添加到UT2014模型中，以产生UT2017模型，该模型复制了包括CH ₂在内的自由基的产生Cl。最后，使用UT2017模型，我们模拟了典型的SiC化学气相渗透条件下的气体成分，主要包括MTS和H ₂。在我们先前的报告中，将模拟结果与成膜物质的分压进行了比较，结果表明，CH ₂ SiCl ₃是MTS / H ₂可能是SiC的成膜物质。为了进行定量验证，我们在考虑CH ₂ SiCl ₃的消耗量的同时估算了反应堆中CH ₂ SiCl ₃的分压分布。在SiC表面上。对于反应堆中所有位置，该模拟结果的值几乎与我们的实验结果相同。因此，我们定量地表明CH ₂ SiCl ₃是SiC的成膜物质。