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.
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