Pulsed laser preparation and quantum superposition state evolution in regular and irregular systems

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Abstract
The nature of the prepared state is crucial to an understanding of isolated-molecule intramolecular dynamics. A model is utilized to compare the created quantum superposition state in pulsed laser excitation from (1) a ground electronic state with regular nuclear wavefunctions to an excited electronic state with regular nuclear wavefunctions with that from (2) the regular ground state to an excited state with irregular nuclear wavefunctions. All results are in the quantum-mechanical small-molecule limit. Visual inspection of the created state and its evolution shows distinct qualitative differences in these two cases, although various theoretically studied quantities do not reveal an obvious distinction. The differences are expected to be experimentally observable in time-resolved emission.