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