Intramolecular vibrational energy relaxation. Decomposition of chemically activated alkylcyclobutanes

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Abstract
This paper describes an approach to the study of intramolecular energy relaxation of highly vibrationally excited complex molecules. The features of the decomposition of a series of chemically activated alkylcyclobutanes are outlined, including variable selectivity of the initial, non-randomized state of excitation. It is shown how this can afford both a qualitative test of the postulate of internal energy randomization employed in the Rice–Ramsperger–Kassel–Marcus treatment of unimolecular reactions, as well as a quantitative measure of the rate of relaxation. The study of the first members of this series, ethyl and dimethyl cyclobutane, is described. As expected, the first members can provide a lower limit to the relaxation rate, namely, λ > 1012 s−1.

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