Thomas E. Markland

Accurate and efficient ground and excited state quantum dynamics by exploiting inherent time and lengthscales: from photoinduced electron transfer to enzyme catalysis.

The development of methods that can treat nonadiabatic quantum dynamics in condensed phase atomistic environments remains a significant challenge in problems ranging from exciton transport in photovoltaic materials to electron and proton transfer in catalysis. In this talk I will discuss our recent developments that allow for the accurate and efficient inclusion of quantum structure and dynamics on ground and excited states by exploiting the inherent time and length-scales in condensed phase systems. For ground state surfaces I will outline how our methods now allow us to perform ab initio path integral simulations that incorporate the quantum nature of the electrons and nuclei at a computational cost as low as treating the nuclei classically. I will then show how one can obtain dramatically improved accuracy in excited state dynamics by combining semiclassical methods with the exact generalized quantum master equation formalism. The utility of these approaches will be illustrated with recent applications ranging from photoinduced electron transfer to enzyme catalysis.