Quasiperiodic and Stochastic Behavior in Molecules

The extent and rate of intramolecular energy transfer play a role in a variety of problems in chemical dynamics. Examples are unimolecular reactions (1 a,b), chemical activation (2a,b), vibrational-rotational-translation energy distribution of the products of a dissociating species (3, 4), infrared multiphoton decomposition of molecules (5a,b, 6), internal conversion and intersystem crossing of electronically excited states (7a-d), dissociation of vibrationally excited state-selected van der Waals complexes (8), fluorescence spectra of electronically and vibrationally excited molecules (9a,b, 10a,b), chemiluminescent spectra of vibrationally excited molecules (11), reactions induced by excitation of high overtones of a bond vibration (12a-c), and high overtone spectra (13a,b). The present article reviews recent theoretical studies on the quasiperiodic and chaotic dynamical aspects of vibrational states and describes how those studies may be related to intramolecular randomization