Quantum dynamics from classical trajectories: New approaches to simulating biological and molecular photocatalysts

Abstract

We will describe new path-integral methods for the direct simulation of condensed-phase electron transfer, proton transfer, and proton-coupled electron transfer (PCET) reactions [1]. Specific topics will include (i) direct simulation PCET reaction mechanisms and rates in iron bi-imidazoline systems across multiple regimes [2,3] and (ii)recent progress in simulation of multi-electron processes.[1] Habershon S, Manolopoulos DE, Markland TE, and Miller TF, "Ring polymer mol. dynamics: Quantum effects in chem. dynamics from classical trajectories in an extended phase space," Annu. Chem., 64, 387 (2013).[2] Warren JJ, Menzeleev AR, Kretchmer JS, Miller TF, Gray HB, and Mayer JM, "Long range proton-coupled electron transfer reactions of bis(imidazole) iron tetraphenylporphyrins linked to benzoates," J. Lett.,4, 519 (2013).[3] Kretchmer JS and Miller TF, "Direct simulation of proton-coupled electron transfer across multiple regimes," J. Phys., in press.