The role of laser-pulse phases in the sub-picosecond optimal infrared multiphoton dissociation of HF

In a simulation of the five-pulse, subpicosecond, optimal infrared multiphoton dissociation of an HF molecule (M. Kaluža, J.T. Muckerman, P. Gross and H. Rabitz, J. Chem. Phys. 100 (1994) 4211), randomizing phases of an optimal pulse reduced the dissociation yield by nearly a factor of two. Here we simulate the response of an HF molecule to ten five-laser pulses which lack shot-to-shot phase reproducibility. We optimize the timings and carrier frequencies of the five pulses to achieve the maximal average dissociation yield over the ensemble of shots, and provide an estimate for the yield in an experiment in which phases of the laser pulses are not controllable.