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Center for Nonlinear Studies |
Better understanding of excited-state charge and energy transfer processes is essential for the rational design of devices for efficient solar energy conversion and solar fuel production. Because electrons respond on a faster timescale to photo-excitation than nuclei, the molecular system is placed in a non-equilibrium configuration, requiring molecular dynamics simulations to describe relaxation and charge and energy flow within the system. Born-Oppenheimer (or adiabatic) molecular dynamic assumes nuclear and electronic motions are not directly coupled, meaning the trajectories of nuclei can be propagated on a single potential energy surface; however, when a molecule is in an excited state, multiple potential energy surfaces may cross at regions of strong nonadiabatic coupling requiring special treatment to incorporate quantum effects into the nuclear dynamics. Recently a generalization of Gaussian wavepacket dynamics has been developed which allows for the coupling of nuclear wavepackets on different adiabatic surfaces for conducting nonadiabatic dynamics simulations. So far this method has only been applied to model systems. The goal of my current work is to extend the application of the coupled wavepacket algorithm to the study of excited-state energy transfer in molecular systems.
Host: Chris Neale