Theory of Laser-Pulse-Induced Molecular Dynamics: Gas-Phase Molecular Collisions and Adbond Dynamics

摘要

A semiclassical study presented here indicates that a sufficiently short and intense pulse can be much more effective in inducing a collisional radiative transition than cw radiation or a long pulse, although the intensity must not be too high because the Rabi oscillation can bring down the probability. For the situation of a molecule physisorbed on a crystalline surface and irradiated by a laser, a master equation approach, used to describe the time evolution of the population of the vibrational adbond levels, shows that for high intensities, laser induced vibrational excitation is the same for pulsed and cw lasers. Keywords: Molecular dynamics, Laser induced, Short pulses, Molecular collisions, Electron transitions, Desorption, Reprints. (jhd)