An Ab Initio RRKM/Master Equation Investigation of SiH_4 and GeH_4 Decomposition Kinetics Using a Kinetic Monte Carlo Approach

摘要

The unimolecular decomposition reactions of SiH_4 and GeH_4 are among the most important gas phase processes active during the CVD of Si and Ge. Despite of this, only few studies are available in the literature on their kinetics. In this work we investigated the decomposition of SiH_4 and GeH_4 by solving the master equation using a stochastic kinetic Monte Carlo approach. RRKM microcanonical kinetic constants were determined using classic and microcanonical J-resolved variational transition state theory adopting high level ab initio data. The simulation results agree well with experimental data for the decomposition of SiH_4 and GeH_4, which were found to be deep in their fall off regime even at atmospheric pressure at typical Si and Ge deposition temperatures.