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Theory and simulation of energy transfer dynamics in van der Waals clusters

An overview of our recent work on the theory and simulation of the vibrational predissociation dynamics of I2(B,v)-Ar13 clusters is given. The decay of the intact cluster induced by vibrational relaxation of the excited impurity exhibits unusual nonexponential behavior, characterized by an instantaneous rate that increases with time. A hybrid statistical model is described, which explicitly takes into account the slow relaxation of the impurity while assuming rapid redistribution of energy among the low frequency cluster modes. This model provides a good description of the statistical dissociation dynamics. A direct mechanism for rapid and selective ejection of rare gas atoms from the system is identified, and understood in terms of correlated binary collisions between molecule and `solvent' atoms facilitated by a nonlinear resonance phenomenon.