Abstract

Results from spectroscopic studies of the vibrational levels of dissociating molecules and from state-selected, state-resolved photofragmentation spectroscopy are presented. The extent of energy flow among the modes of a molecule is explored through the couplings, or lack thereof, revealed by high-resolution spectroscopy. The dynamics of energy flow during bond breaking are revealed by photofragment excitation spectroscopy and by product energy state distributions. These completely resolved data provide sensitive tests of dynamical constraints such as vibrational or rotational adiabaticity and thus of theoretical models for unimolecular reaction dynamics.

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