We investigate two classes of quantum control problems by using frequency-domain optimization algorithms in the context of ultrafast laser control of quantum systems. In the first class, the system model is known and a frequency-domain gradient-based
optimization algorithm is applied to searching for an optimal control field to selectively and robustly manipulate the population transfer in atomic Rubidium. The other class of quantum control problems involves an experimental system with an unknown model. In the case, we introduce a differential evolution algorithm with a mixed strategy to search for optimal control fields and demonstrate the capability in an ultrafast laser control experiment for the fragmentation of Pr(hfac)$_3$ molecules.
Exploring molecular breakup processes induced by light-matter interactions has both fundamental and practical implications. However, it remains a challenge to elucidate the underlying reaction mechanism in the strong field regime, where the potential
s of the reactant are modified dramatically. Here, we perform a theoretical analysis combined with a time-dependent wavepacket calculation to show how a strong ultrafast laser field affects the photofragment products. As an example, we examine the photochemical reaction of breaking up the molecule NaI into the neutral atoms Na and I, which due to inherent nonadiabatic couplings is indirectly formed in a stepwise fashion via the reaction intermediate NaI. By analyzing the angular dependencies of fragment distributions, we are able to identify the reaction intermediate NaI from the weak to the strong field-induced nonadiabatic regimes. Furthermore, the energy levels of NaI can be extracted from the quantum interference patterns of the transient photofragment momentum distribution.
