Molecular Dynamics Study of Light-Harvesting Molecules with Electronic Transition

Harvesting energy from sunlight is of paramount importance for the so-lution of the global energy problem, for which synthetic supermolecules such as light-harvesting dendrimers are attracting great attention. In these molecules, electronic excitation energy due to photoexcitation of antennas located on the periphery of the molecules is rapidly transported to the photo-chemical reaction centers at the cores of the molecules, which in turn perform useful work such as photosynthesis and molecular actuation [1]. Though such energy transfer is conventionally attributed to either dipole-dipole interac-tions (Forster mechanism) or the overlapping of donor and acceptor electronic wave functions (Dexter mechanism), atomistic mechanisms of rapid electron transport in these dendrimers remain elusive. In order to identify atomistic mechanisms of rapid energy transport af-ter photoexcitation of a light-harvesting dendrimer, we perform quantum-mechanical molecular dynamics simulations. To incorporate nonadiabatic electronic transitions, the fewest-switches surface-hopping (FSSH) metho