Quantum Dynamics and Spectroscopy of Reactive Species in Heterogeneous Environments

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Professor Thomas Markland of Stanford University is supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry to develop theoretical and computational methods to treat reactive chemical processes that occur in disordered materials such as those found at electrochemical interfaces, in nanojunctions, and biological proton channels. Describing these processes requires the ability to accurately capture the quantum mechanics of both the electrons and nuclei in these disordered systems and to connect them to experimental approaches, such as ultrafast spectroscopies, that are now providing new hints into the mechanisms underlying these processes. Markland’s research will provide new theoretical methods and algorithms that can be used by the chemistry, biochemistry, and materials science communities and will be implemented in widely used software packages.Professor Thomas Markland and his research team are developing methods to accurately simulate and elucidate the quantum mechanics of both the electrons and nuclei in disordered molecular systems and link them to experimental approaches, such as ultrafast spectroscopies. They are achieving this by: (i.) introducing approaches to accurately obtain diabatic electronic surfaces and electronic couplings for electron transfer processes between molecules in solution and solid (metal or semiconductor) interfaces, (ii.) developing quantum dynamics approaches to treat systems coupled to molecular environments such as electrode surfaces, (iii.) devising schemes to improve the accuracy of machine-learned potential energy surfaces trained to model reactive defects, and (iv.) providing the theory to efficiently construct the signals obtained from multidimensional spectroscopies. Together these advances will improve our ability to capture the quantum dynamics and electronic structure of processes involving proton defect and electron transport that are essential to elucidate cutting edge experiments and design more efficient materials for interfacial catalysis and mesoscopic transport.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.