Impulsive effects of phase-locked pulse pairs on nuclear motion in the electronic ground state

The nonlinear effects of ultrashort phase-locked electronically resonant pulse pairs on the ground state nuclear motion are investigated theoretically. The pulse-pair propagator, momentum impulse, and displacement are determined in the weak field limit for pulse pairs separated by a time delay short on a nuclear time scale. Possible application to large amplitude vibrational excitation of the 104 cm−1 mode of α-perylene is considered and comparisons are made to other Raman excitation methods.