Abstract
Abstract A model description of vibrational relaxation (redistribution) (VR) in the quasicontinuum (QC) of polyatomic molecules, subject to infrared multiphoton excitation (IR MPE) has been introduced, based on the kinetic equations technique. This model has been applied to the derivation of expressions for the population distributions as well as dissociation quantum yields (QYs) of polyatomic molecules under IR MPE, with special emphasis on the dependence of the obtained QYs on exciting laser pulse intensity and duration as compared to the VR rate constant. Good agreement has been obtained between the theoretically derived dependences of the dissociation QYs in SF 6 on buffer gas pressure and experimental data.
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