Molecules in Classical and Quantized Fields: Improving Time-Dependent Density Functional Approximations and Correlated Electron-Ion Methods

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Professor Neepa Maitra of Hunter College, City University of New York (CUNY) is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. Dr. Maitra and her research group develop new methods for simulating the behavior of molecules exposed to light. Understanding and computationally modeling the motion of electrons and ions in molecules and solids far from their stable, equilibrium states is necessary for understanding photovoltaic processes, photocatalysis, radiation damage in biomolecules, nanoscale conductance devices, time-resolved pump-probe spectroscopies, and the production of compact light sources. Dr. Maitra's group develops theoretical methods from first-principles for computational simulations to reliably and efficiently predict these processes. Dr. Maitra organizes mini-workshops in electronic structure and dynamics open to the wider New York/New Jersey area. She trains undergraduate and graduate students in cutting-edge research and uses innovative peer instruction teaching techniques in her undergraduate classes.Dr. Maitra and her research group are developing new methods for the correlated dynamics of electrons, ions, and photons, in three aims. In one aim, improved functional approximations for time-dependent density functional theory (TDDFT) in the non-perturbative regime is derived. This is built on an exact expression for the exchange-correlation potential. This research moves TDDFT towards use in real-time dynamics as confidently as DFT is used for ground-state properties. In the second aim, practical mixed quantum-classical methods based on the exact factorization approach for correlated electron-ion dynamics in laser fields are being constructed that include electronic decoherence and wave packet branching from first-principles. The third area extends exact factorization to light-matter systems to gain a fundamental understanding of how field quantization can alter and control chemical reactions, as well as to develop practical mixed quantum-classical methods for the dynamics and control of molecules in cavities. The research impacts topical applications where knowledge and understanding beyond ground-state electronic structure is needed, including photovoltaic design, and quantum control of electronic and nuclear dynamics by attosecond or femtosecond laser fields, or by tuning cavity parameters in polaritonic chemistry.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.