First-Principles Excited State Electronic Dynamics

华盛顿大学的李晓松获得了化学学部化学理论、模型和计算方法项目的奖励，他开发了几种随时间变化的电子结构方法，并结合严格的分析方法来解决一些特定的、重要的受激电子动力学与环境相互作用的系统。拟议的研究计划建立在LI小组在第一原理电子动力学领域已经取得的成就之上。总体目标是开发新的方法，能够解决受激电子动力学与分子自由度和溶剂的时间依赖相互作用。这些新方法使李和他的同事们能够探索新的、有趣的现象，其精确度和细节都能满足前沿实验的需要。具体来说，他们计划应用这些新方法来研究有机和无机材料中振动诱导的电子-空穴对弛豫、溶剂诱导的激发态衰减和溶剂调制的激发态反应途径。从这些研究中获得的基础知识加深了对有机和无机材料中许多相关光物理过程的理解。激发态电子动力学在能量转换、能量存储、光催化以及信息处理和存储中无处不在。它们是许多未来技术的核心，尤其是在光子学和自旋电子学领域。从拟议的研究中获得的知识通过改变研究人员理解激发态电子结构/功能关系的方式，对这些技术具有广泛的影响。该项目可能进一步导致具有新型光物理特性的新材料的开发，用于从基础研究到能量转换的各种科学背景。该项目的结果为化学和物理中激发态与环境的相互作用提供了新的基本见解。该研究为无机化学、理论化学、物理化学和材料化学领域的高级跨学科教育和培训提供了一种机制，以便为参与研究的本科生和研究生将来在科学、工程和教育领域的职业做好准备。

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.