Abstract
A theory for van der Waals molecules (AB---C) is presented, which is based on the concept that a van der Waals molecule can be considered as a nonrigid molecule because it is loosely bound in comparison with proper chemical bonds. A perturbation method is performed for the three-body internal Hamiltonian which has been obtained for the case in which the angular momentum of the whole molecular system is equal to zero (J=0). A new idea, the dynamic perturbation mechanism of vibrational energy transfer, is presented which originates in the coupling of the kinetic energy of the chemical and van der Waals bonds. This is applied to the vibrational predissociation process of the van der Waals molecule and linewidths and lifetimes are calculated by estimating the dynamic coupling. The decay rates calculated by this new mechanism are quite large and are comparable to those values estimated by the usual treatment of the perturbation potential.
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