We investigate the extent to which unidirectional intramolecular torsional motion can be created in an oriented bicyclic model system driven solely by laser light. We apply the machinery of quantum control via specifically tailored laser pulses to induce such motion, eliminating the need for the thermally constrained steps conventionally used in molecular motor systems. Our approach does not rely on specific details of the potential surfaces to create a preferred direction. Rather, we use matter-field interaction and the tools of coherent optimal control to create a wave packet with nonzero angular momentum among unbound torsional states on an excited electronic surface. Analysis of the results of the control algorithm provides general insight into when and how optimal control theory can find solutions that could not be generated through simple intuitive schemes. We find that, under constrained polarization, the control algorithm reduces to a simple intuitive coherent control strategy wherein a first IR pulse creates a non-stationary wave packet on the ground surface and a subsequent UV pulse transfers it to the excited state. Allowing for polarization shaping, however, we find new control routes that go beyond the intuitive scheme.
ASJC Scopus subject areas
- Physics and Astronomy(all)