Analysis of femtosecond quantum control mechanisms with colored double pulses

Fitness landscapes based on a limited number of laser pulse shape parameters can elucidate reaction pathways and can help to find the underlying control mechanism of optimal pulses determined by adaptive femtosecond quantum control. In a first experiment, we employ colored double pulses and systematically scan both the temporal subpulse separation and the relative amplitude of the two subpulses to acquire fitness landscapes. Comparison with results obtained from a closed-loop experiment demonstrates the capability of fitness landscapes for the revelation of possible control mechanisms. In a second experiment, using transient absorption spectroscopy, we investigate and compare the dependence of the excitation efficiency of the solvated dye molecule 5,5(')-dichloro-11-diphenylamino-3,3(')-diethyl-10,12-ethylene thiatricarbocyanine perchlorate (IR140) on selected pulse shapes in two parametrizations. The results show that very different pulse profiles can be equivalently adequate to maximize a given control objective. Fitness landscapes thus provide valuable information about different pathways along which a molecular system can be controlled with shaped laser pulses.