Abstract

A model is presented for the vibrational population relaxation of a polyatomic molecule in solution. The coupling of molecular vibrations leads to a cascade of energy through a sequence of vibrational levels. At each step of the energy redistribution energy can be transferred to nonvibrational (solvent) degrees of freedom. The model is developed in detail for a two step cascade, incorporating variable coupling potentials between zero order vibrational and solvent eigenstates. The results of these calculations are discussed in the context of time resolved picosecond laser studies of vibrational relaxation in liquids.

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