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Time-independent [Halberstadt and co-workers, J. Chem. Phys. 96, 2404 (1992); 97, 341 (1992)] and time-dependent quantum mechanical calculations that describe the intramolecular vibrational relaxation (IVR) of Ar⋯Cl 2 are used to develop analytical models for this process. It is shown that time-resolved experiments should reveal an oscillatory dissociation rate. It is found that the oscillations will be different for different rotational levels, and may tend to wash out if insufficient state selection is achieved in the initial excitation step. This may explain why no such oscillations were observed for Ar⋯I2. It is also predicted that the observed product state rotational distribution will change with the initially excited rotational state. © 1993 American Institute of Physics.N. H. and K. C. J. wish to acknowledge support by the CNRS-NSF international collaboration program. This work was partially supported by CICYT Grant No. PB87- 0272 and by the Comunidad Aut6noma de Madrid Grant No. 064/92.Peer Reviewe

Coherence effects between intramolecular vibrational relaxation and dissociation in triatomic van der Waals systems