Picosecond Chemistry of Collisionless Molecules in Supersonic Beams

Abstract

The dynamics of collisionless intramolecular vibrational-energy redistribution (IVR), bond breakage, and bond formation in large isolated molecules is currently a very important and challenging problem. A fruitful approach to this problem involves the study, via direct measurements in the time domain, of the decay parameters of energetically excited molecules. Using such an approach one can determine unimolecular rate constants as well as study any quantum mechanical coherence phenomena that may be involved in a decay process. Furthermore, in cold beams these rates and coherence effects can be studied as a function of the energy and character of individual vibrational modes in a molecule. The results of such studies are important to understanding the nature of energy flow within molecules and to assessing the possibility of vibrational mode-selective laser chemistry [1].

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