CAREER: Coupled electronic and nuclear dynamics in organometallic enzymes and photocatalysts

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Thomas Miller of the California Institute of Technology is supported by an award from the Theory, Models and Computational Methods program in the Chemistry division to develop new theoretical methods to understand coupled electronic and nuclear dynamics in organometallic catalysts and photocatalytic enzymes. These methods are designed to overcome the intrinsic challenges of simulating and understanding the dynamics of processes that are central to solar photocatalysis, including long range electron transfer dynamics in proteins, redox-coupled proton transfer dynamics, and multiple electron transfer events in enzymes. The work has two objectives:1) Reducing many-electron problems to few-electron problems in large-scale systems by developing a general embedded density functional theory (e-DFT) approach to obtain reduced descriptions for the electronic structure of large-scale systems. 2) Obtaining new insights into proton-coupled electron transfer (PCET) dynamics by combinging the ring-polymer molecular dynamics (RPMD) method with the e-DFT approach to simulate reaction dynamics in photcatalysts and enzymes.The rational design of molecular photosystems is a challenge of paramount scientific, industrial, and societal importance. Computational research has the potential to make extraordinary contributions in this area by allowing for detailed investigations of biological photosystems, by revealing key insights into fundamental photochemical processes, and by allowing for fast and inexpensive screening of synthetic photocatalysts. Prof. Miller and his research group are also engaged in a novel outreach effort, the TRIDENT Program - Team Research yielding Integrated Educational Tools. TRIDENT is a three-stage program in which (i) a team composed of the PI, a local high-school student, and local science teacher collaborates on a computational summer research project, (ii) using skills and ideas developed through the research, the team tailors a plan to integrate computational research software into the teacher?s classroom, and (iii) the PI visits the classroom to gain feedback on the implementation of the plan, to refine the plan, and to discuss careers in science. TRIDENT provides sustainable educational support to teachers and students at local public schools.