Assembling gas-phase reaction mechanisms for high temperature inorganic systems based on quantum chemistry calculations and reaction rate theories

Detailed chemical kinetic modeling based on computational quantum chemistry has been quite successful in making quantitative predictions about some systems, particularly the combustion of small hydrocarbons and certain areas of atmospheric chemistry. The gas phase chemistry of many processes in high-temperature inorganic systems, from materials synthesis to propulsion to waste incineration, could in principle be modeled with equal or greater success using detailed chemical kinetic modeling. This contribution provides examples from our own work of how computational quantum chemistry can be used in developing gas phase reaction mechanisms for modeling of high temperature materials processing. In the context of CVD of silicon from dichlorosilane, CVD of alumina from AlCl3/H2/CO2 mixtures, and particle nucleation from silane, this detailed chemical kinetic modeling has given us insight into gas phase reaction pathways that we would not likely have gained by other means. q 2004 Elsevier Ltd. All rights reserved. keywords: Chemical kinetics; Quantum chemistry; Reaction mechanism; Silicon; Aluminum; ab initio