Coherent control through near-resonant Raman transitions

Abstract

The phase of an electronic wave function is shown to play an important role in coherent control experiments. By using a pulse shaping system with a femtosecond laser, we explore the phase relationships among resonant and off-resonant Raman transitions in Li{sub 2} by measuring the phases of the resulting wave packets, or quantum beats. Specific pixels in a liquid-crystal spatial light modulator are used to isolate the resonant and off-resonant portions of the Raman transitions in Li{sub 2}. The off-resonant Raman transitions have an approximately 90 degree sign phase shift with respect to the resonant Raman transition, and there is an approximately 180 degree sign phase shift between the blue-detuned and the red-detuned off-resonant Raman transitions. Calculations using second-order time-dependent perturbation theory for the electronic transitions agree with the experimental results for the laser pulse intensities used here. Interferences between the off-resonant Raman transitions as a function of detuning are used to demonstrate coherent control of the Raman quantum wave packet.