Abstract

A theoretical study of radiative transitions in molecular collisions occurring in the presence of short laser pulses is carried out within the semiclassical two-state formalism. Transition probabilities are calculated by numerically integrating the Bloch equation for two model systems and the Na-Ar system. At high laser intensities where a short pulse is more effective in inducing transitions than cw radiation, the transition probability exhibits nonlinear character with respect to the pulse intensity. At such high intensities, noncollisional atomic transitions may also be present, which need to be eliminated for an observation of collisional transitions.

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