IMPULSIVE EFFECTS OF PHASE-LOCKED PULSE PAIRS ON NUCLEAR MOTION IN THE ELECTRONIC GROUND-STATE

The nonlinear effects of ultrashort phase-locked electronically resona nt pulse pairs on the ground state nuclear motion are investigated the oretically. The pulse-pair propagator, momentum impulse, and displacem ent are determined in the weak field limit for pulse pairs separated b y a time delay short on a nuclear time scale. Possible application to large amplitude vibrational excitation of the 104 cm-1 mode of alpha-p erylene is considered and comparisons are made to other Raman excitati on methods.