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Rate constants and expressions for the initial processes in the decomposition of ethanol have been derived on the basis of existing experimental and estimated results. Energy transfer effects on the multichannel decomposition processes have been determined through the solution of the master equation and on the basis of exponential‐down and step‐ladder collisional transition models. The predominant (lower threshold) channel is unaffected by the presence of the upper channels and results for the two transition models can be brought into correspondence by using a somewhat higher value for the step‐size down parameter in the step‐ladder model. For the upper channels and with an exponential‐down model, the logarithms of the ratio of the rate constants between perturbed and unperturbed systems can be captured by a sigmoidal shaped curve. In the case of the step‐ladder model, the logarithms of this ratio decreases monotonically. Initially, differences between the two models are small (after adjusting the step‐size down parameter). The results are compared with the recent simulations of Marinov. The order of magnitude differences in rate constants have been traced to the inclusion in the present study of experimental results pertaining to decomposition and the reverse combination processes in addition to the proper treatment of energy transfer effects during multichannel decompositions. Some observations regarding the parameterization of this type of pressure dependent data for use in simulations are presented. © 2004 Wiley Periodicals, Inc. Int J Chem Kinet 36:456–465, 2004.
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