Hybrid quantum/classical simulation and kinetic study of the vibrational predissociation of Cl-2 center dot center dot center dot Ne-n (n=2, 3)

A hybrid quantum/classical method is applied to the vibrational predissocia tion of van der Waals clusters containing a diatomic molecule and several r are gas atoms, Cl-2... Ne-n (n=2, 3). The vibrational degree of freedom of the diatomic is treated quantum mechanically while all the other degrees of freedom are treated classically. A kinetic mechanism is proposed in order to interpret the dynamics in terms of the following elementary steps; vibra tional predissociation (VP), intramolecular vibrational redistribution (IVR ), and evaporative cooling (EC). The resulting lifetimes are in very good a greement with the experimental linewidth measurements of Janda and co-worke rs, and with the quantum mechanical reduced-dimension results of Le Quere a nd Gray on Cl-2... Ne-2. The final rotational state distributions agree ver y well with the experimental results and exhibit a quasistatistical behavio r. The final vibrational distributions reproduce the main experimental feat ures. (C) 1999 American Institute of Physics. [S0021-9606(99)01733-X].