Mixed Quantum Classical Simulations of Charge-Transfer Dynamics in a Model Light-Harvesting Complex. I. Charge-Transfer Dynamics.

We develop here a mixed quantum mechanical/molecular dynamics model to investigate charge-transfer dynamics in a set of large organic donor-bridge-acceptor triad molecules. Specifically, we are interested in the differences in electron and nuclear behavior relating to small changes in the molecular makeup of carotenoid-porphyrin-fullerene triads. Our model approximates excitation energies on the order of 1.9 eV which agree with absorption spectra for these triads and isolated porphyrins. Using electron population analysis, we monitor charge migration to the acceptor in time. Approximations of the charge transfer rates reveal ultrafast (picosecond scale) electron dynamics consistent with experimental literature.