Theoretical optimization and prediction in the experimental search space for vibrational quantum processes

Control and optimization prospects in the frequency domain are studied theoretically, using a genetic algorithm (GA) and shaping Fourier-limited (FL) pulses. The objectives are state-to-state transitions and unitary transformations, within the scope of vibrational excitation of transition metal carbonyls. In analogy to experimental closed-loop setups, two different implementations of the phase function are investigated: a free phase variation and a sinusoidal phase modulation. We examine the control landscape generated by the parametrized phase functions and clarify the underlying mechanism. Strategies to decrease the complexity of the laser fields are developed, benefiting from previous optimal control theory calculations. Additionally, we pass the capabilities of the experiment and optimize the FL pulses with the GA simultaneously to the phase and transmittance functions. This allows us to predict promising FL-pulse properties and mask functions for future experiments.