Nonperturbative quantum control via the nonresonant dynamic Stark effect

The nonresonant dynamic Stark effect (NRDSE) is investigated as a general tool for quantum control in the intermediate field strength regime (nonperturbative but nonionizing). We illustrate this scheme for the case of nonadiabatic molecular photodissociation at an avoided crossing. Using the NRDSE exclusively, both the electronic branching ratio and predissociation lifetime may be controlled. Infrared control pulses are used to modify the field-free dynamical evolution during traversal of the avoided crossing, thus controlling the nonadiabatic branching ratio. Predissociation lifetimes may be either increased or decreased using properly timed short infrared pulses to modify phase differences between the diabatic wave packets. In contrast with the limiting cases of perturbative control (interference between transitions) and strong field control with ionizing laser fields, control via the NRDSE may be thought of as reversibly modifying the effective Hamiltonian during system propagation.