PROJECT OUTCOMES REPORT

The accurate prediction of excited-state electronic structure and dynamics from first principles is crucial to attaining a detailed mechanistic understanding of the light-matter interactions that drive the fundamental processes implicated in energy conversion, energy storage, and photocatalysis.  Excited-state electronic structure methods have ushered in an era of rational design for advanced functionalized materials and hold the promise of expediting the development of many proposed and emerging technologies, most notably in the areas of photonics and spintronics as they apply to information processing and storage. The primary goal of this project is to provide accurate and reliable guidance for experimentalists through furthering the development and application of theoretical/computational chemistry.  In order for the application of quantum mechanics to molecular systems to be simultaneously predictive, accurate and tractable, innovative advances in computer software and mathematical algorithms are demanded.  The computational/theoretical tools developed in our group as well as the chemical systems to which they are applied are experimentally motivated, and largely focus on modeling excited state electronic structures and the way these nonequilibrium electronic configurations evolve in time. The PI's independent research at the University of Washington supported by this award can be categorized into two broad and coherently integrated research areas:

(i) method developments, including first-principles electronic dynamics and Ehrenfest dynamics using real-time, time-dependent density functional theory; near-linear scaling methods for optimizing molecular geometries and excited state electronic wave functions;

(ii) scientific applications, including understanding the physical underpinnings of exotic  electric/magnetic interactions among charger carriers in diluted magnetic semiconductors; laser-controlled molecular reactions; electron-hole and charge transfer dynamics in organic materials and semiconductor nanocrystals; and optical properties of organic chromophores.

The information gleaned from the proposed research has broad implications for each of these technologies by providing researchers a deeper understanding of the excited state electronic structure/function relationships. This project furthermore results in the development of new materials with novel photophysical properties for application in a variety of scientific contexts from fundamental research to energy conversion. Finally, this research provides new fundamental insights into interactions of excited electronic states and environments in chemistry and physics, and will deepen our understanding of this important class of interactions. This project is transformative in that it yields new chemical strategies for controlling excited state dynamics and also provides new theoretical approaches to analyze the electronic structure origins of these dynamics.

The research also provides a mechanism for advanced interdisciplinary education and training in the areas of inorganic, theoretical, physical, and materials chemistries, in order to prepare participating students for future careers in science, engineering, and education. Students collaborate with experimental researchers at international universities, and participate in UW's interdisciplinary educational programs, providing them with invaluable exposure to other research experiences and scientific cultures. Special emphasis has been placed on integration of research and education at the undergraduate and high school level through (a) extensive involvement of undergraduates in the scientific research, (b) incorporation of experiments and concepts from the proposed research into the UW undergraduate physical chemistry curriculum, (c) collaboration with the UW A...

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