January 1, 1974Journal of the Chemical Society Faraday Transactions 2 Molecular and Chemical Physics27 citations
Theory of intramolecular vibrational relaxation in large systems
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Abstract
A general theory for intramolecular vibrational relaxation is proposed. The theory provides a master equation, analogous to the Pauli master equation in non-equilibrium statistical mechanics, for this process. The master equation contains a completely general time independent perturbation operator, which causes the system to relax to equilibrium. The choice of the three-phonon interaction operator as a perturbation is treated in detail, and a comparison with experimental data is made.