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Full-dimensional quantum dynamics calculations on ArI2(B,vi) vibrational predissociation with total angular momenta J=0, 1, and 2 are presented. Models based on a few interacting states are shown to reproduce important aspects of the dynamics, confirming that vibrational predissociation is mediated by a few-state intramolecular vibrational energy redistribution effect. As a consequence, vibrational predissociation rate constants exhibit large oscillations with vi, the initial I2 vibrational quantum number in the complex. The qualitative effect persists when alternative choices for the interaction potential parameters are considered. Similarly, despite the importance of Coriolis coupling, the effect persists as J is varied from 0 to 2. We also discuss how the effect may be difficult to observe in typical experiments that involve higher J values. © 1996 American Institute of Physics.O.R. was supported by DGICYT Grant No. PB92-0053. S.K.G. was supported by the Ofce of Basic Energy Sciences, Division of Chemical Sciences, U.S. Department of Energy under Contract No. W-31-109-ENG-38.Peer Reviewe

Quantum dynamics of ArI2 vibrational predissociation including low total angular momenta: The role of intramolecular vibrational energy redistribution