Abstract
Experiments involving laser-induced hot bands have interrogated the energies and populations of ground-state vibrational levels of perylene. In the bare molecule, many ground-state levels persist into the 10 -7 -10 -6 -s regime without significant relaxation. Even in the perylene/Ar 1 van der Waals complex, a ground-state quantum of 353 cm -1 persists for >120 ns. On the other hand, residual collisions in the expanding free jet cause significant relaxation of energy deposited in low-energy (G) modes of perylene. Hot bands of free perylene are also generated following vibrational predissociation of van der Waals complexes
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