New approaches to simulating biological and molecular catalysts

Abstract

A primary focus of our research is the development of dynamics simulation methods that reveal the mechanistic details of quantum mech. reactions that are central to biol. and mol. catalysis. The nature of this effort is three-fold: firstly, we work from the foundation of quantum statistical mechanics and semiclassical dynamics to develop path-integral methods that expand the scope and reliability of condensed-phase quantum dynamics simulations. Secondly, we develop quantum embedding methods to improve the description of mol. interactions in systems with subtle electronic properties. And finally, we apply these methods to the mechanistic features of condensed-phase systems, including enzyme reactions and inorg. electron-transfer and protoncoupled electron transfer (PCET) processes. In the talk, we will describe these theor. approaches and their application to chem. reactions. We will particularly focus on the recent development of path-integral methods for the description of general, non-adiabatic reactions and the application of this approach to biol. charge transfer.