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Semiclassical treatment of time-dependent molecular dynamics

A semiclassical expression for the total final-state probability of one-photon-resonant two-photon excitation of a diatomic molecule by two time-delayed short laser pulses is derived. It is in good agreement with numerical results and clearly exhibits the dependence of this quantum mechanical observable on the lineshapes of both laser pulses and on the classical quantities which characterize the motion of the vibrational wavepacket generated.