Abstract
This study presents simulations of optimal field-free molecular alignment and rotational population transfer (starting from the J = 0 rotational ground state of a diatomic molecule), optimized by means of laser pulse shaping guided by evolutionary algorithms. Qualitatively different solutions are obtained that optimize the alignment and population transfer efficiency to the maximum extent that is possible given the existing constraints on the optimization due to the finite bandwidth and energy of the laser pulse, the finite degrees of freedom in the laser pulse shaping and the evolutionary algorithm employed. The effect of these constraints on the optimization process is discussed at several levels, subject to theoretical as well as experimental considerations. We show that optimized alignment yields can reach extremely high values, even with severe constraints being present. The breadth of optimal controls is assessed, and a correlation is found between the diversity of solutions and the difficulty of the problem. In the pulse shapes that optimize dynamic alignment we observe a transition between pulse sequences that maximize the initial population transfer from J = 0 to J = 2 and pulse sequences that optimize the transfer to higher rotational levels.
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