A study of the reaction dynamics of proton coupled electron transfer (PCET) in model biomimetic photocatalysts is presented. The ring polymer molecular dynamics (RPMD) method for direct simulation of quantum dynamics is combined with rare event sampling techniques to calculate the rate and mechanism for both a fully atomistic and system-bath representation of the PCET reaction present in iron bi-imidazoline complexes. RPMD is a path integral method that provides a trajectory-based formalism to include quantum effects using classical equations of motion. The ensemble of reactive RPMD trajectories is analyzed for both concerted and stepwise pathways elucidating the nature of electron/proton/solvent coupling in PCET reactions.

Direct simulation of proton coupled electron transfer dynamics

243rd National Meeting (2012)

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