Vibrational predissociation of the I2•••Ne2 cluster:: A molecular dynamics with quantum transitions study

The MDQT (molecular dynamics with quantum transitions) method of Tully is applied to the vibrational predissociation of a Van der Waals cluster containing a diatomic molecule and two rare gas atoms, I-2... Ne-2. The vibrational degree of freedom of the diatomic is treated quantum mechanically using DVR (discrete variable representation) while all the other degrees of freedom are treated classically. The results are in very good agreement with the experimentally measured lifetimes and product state distributions. In particular, the final vibrational state distribution of I-2, which could not be satisfactorily reproduced in quasiclassical studies, is well described. Based on these results a different kinetic scheme for interpreting the vibrational predissociation in this system is proposed. In addition, this work shows that the method is very promising for the study of clusters containing more rare gas atoms. (C) 1998 American Institute of Physics. [S0021-9606(98)00839-3].