First-Principles Excited State Electronic Dynamics

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Xiaosong Li of the University of Washington is supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division to develop several time-dependent electronic structure methods in conjunction with rigorous analytical methods to address some specific and important systems of excited electronic dynamics interacting with an environment. The proposed research program builds on what the LI group has already accomplished in the field of first-principles electronic dynamics. The overall objective is to develop new methods that are able to address the time-dependent interactions of excited electronic dynamics with molecular degrees of freedom and solvent. The new methods allow Li and his coworkers to explore new, interesting phenomena with a level of accuracy and detail that meets the needs of cutting-edge experiments. Specifically, they plan to apply the new methods to investigate vibration-induced electron-hole pair relaxation, solvent-induced excited state decay and solvent-modulated excited state reaction pathways in organic and inorganic materials. The fundamental knowledge gained from these studies deepen the understanding of numerous related photophysical processes in organic and inorganic materials. Excited electronic dynamics are ubiquitous in energy conversion, energy storage, and photocatalysis, as well as in information processing and storage. They are central to numerous futuristic, proposed technologies most notably in the area of photonics and spintronics. The knowledge gained from the proposed research has broad implications for each of these technologies by changing the way researchers understand excited state electronic structure/function relationships. This project could furthermore result in the development of new materials with novel photophysical properties for application in a variety of scientific contexts from fundamental research to energy conversion. The results of this project provide new fundamental insights into the interactions of excited electronic states and environments in chemistry and physics. The proposed research provides a mechanism for advanced interdisciplinary education and training in the areas of inorganic, theoretical, physical, and materials chemistry, in order to prepare participating undergraduate and graduate students for future careers in science, engineering, and education.