Theoretical simulations offer an exciting window into chemical reaction dynamics at an atomistic level. Our lab develops and uses techniques based on semiclassical theory and the path integral formulation of quantum theory to investigate quantum mechanical processes in complex chemical systems. Specifically, we focus on characterizing photochemical and thermal charge and energy transfer pathways in the condensed phase, and we use the resulting mechanistic insights to generate design principles for novel materials.
- We develop semiclassical and path-integral based model dynamics to simulate interesting chemistry in the condensed-phase.
- We like methods that are classically isomorphic. We work on developing approximate methods for quantum dynamics that are able to incorporate quantum effects like zero-point energy, tunneling, and coherence and to describe electronically nonadiabatic processes, while retaining the favorable scaling in computational cost with system size exhibited by classical molecular dynamics simulations.
- We seek to understand the molecular origin of chemical selectivity in natural and synthetic systems.
- We are currently investigating exciton chemistry in organic photovoltaics, multi-electron chemistry in tri-metal-center transition metal complexes, and vibrationally promoted hot-electron chemistry in reactions at metal surfaces.
- Our goals are to use a combination of theory, electronic structure, and quantum dynamics to 1) uncover the detailed mechanisms of novel charge and energy transfer phenomena, 2) identify productive reaction pathways/intermediates as well as competing loss mechanisms, 3) isolate significant factors, such as chemical environment, relative geometries, and temperature that determine dominant pathways, 4) construct experimentally verifiable hypotheses to enhance charge/energy transport properties of specific materials, and 5) build a database of transferable design principles that can be used predictively in the development of novel materials.