Coherent Control of Photofragment Distributions Using Laser Phase Modulation in the Weak-Field Limit

The possibility of quantum interference control of the final state distributions of photodissociation fragments by means of pure phase modulation of the pump laser pulse in the weak-field regime is demonstrated theoretically for the first time. The specific application involves realistic wave packet calculations of the transient vibrational populations of the Br2(B, vf) fragment produced upon predissociation of the Ne-Br-2(B) complex, which is excited to a superposition of resonance states using pulses with different linear chirps.

Transient phase effects on the fragment populations are found to persist for long times (about 200 ps) after the pulse is over due to interference between overlapping resonances in Ne-Br-2(B).