Seminar (theoretical): Thomas F. Miller, III, California Institute of Technology
Thomas F. Miller, III - speaker's webpage
Division of Chemistry and Chemical Engineering
California Institute of Technology
Host: Garnet Chan
Quantum Dynamics from Classical Trajectories: Direct simulation of charge transfer in enzymes and molecular catalysts
Condensed-phase charge-transfer reactions are a central feature of many biological and synthetic catalytic pathways. The development of accurate, scalable methods to simulate and understand these reactions is thus a central challenge for chemical theory. In the talk, we will describe recently developed path-integral methods for the direct simulation of condensed-phase electron transfer, proton transfer, and proton-coupled electron transfer (PCET) reactions [1-3]. Specific applications will include (i) characterization of the role of nanometer-scale protein fluctuations in facilitating enzyme-catalyzed hydrogen transfer  and (ii) comparison of concerted vs. sequential reaction pathways for PCET in mixed-valence iron bi-imidazoline systems.
 Miller TF, "Isomorphic classical molecular dynamics model for an excess electron in a supercritical fluid,” J. Chem. Phys., 129, 194502 (2008).
 Ananth N and Milller TF, "Exact quantum statistics for electronically nonadiabatic systems using continuous path variables," J. Chem. Phys., 133, 234103 (2010).
 Menzeleev AR, Ananth N, and Miller TF, "Direct simulation of electron transfer using ring polymer molecular dynamics: Comparison with semiclassical instanton theory and exact quantum methods," J. Chem. Phys., 135, 074106 (2011).
 Boekelheide N, Salomón-Ferrer R, and Miller TF, "Dynamics and dissipation in enzyme catalysis," Proc. Natl. Acad. USA, 108, 16159 (2011).