Optimal control of molecular alignment in dissipative media.

We explore the controllability of nonadiabatic alignment in dissipative media, and the information content of control experiments regarding the bath properties and the bath system interactions. Our approach is based on a solution of the quantum Liouville equation within the multilevel Bloch formalism, assuming Markovian dynamics. We find that the time and energy characteristics of the laser fields that produce desired alignment characteristics at a predetermined instant respond in distinct manners to decoherence and to population relaxation, and are sensitive to both time scales. In particular, the time-evolving spectral composition of the optimal pulse mirrors the time-evolving rotational composition of the wave packet, and points to different mechanisms of rotational excitation in isolated systems, in systems subject to a decoherering bath, and in ones subject to a population relaxing bath.