Accurate Photochemistry in the Condensed Phase

马萨诸塞州理工学院的Troy货车Voorhis获得了理论、模型和计算方法项目的一项奖励，以开发、实施和应用用于模拟复杂环境中光化学过程的变革性工具。特别是，货车Voorhis和他的研究小组专注于扩展基态电子结构理论的技术，以精确处理电子激发态。 他们采用这些新方法来理解三个关键的光化学过程：激发态分子内电子转移（ET），超快荧光光谱和染料的非辐射猝灭。 他们使用约束密度泛函理论（DFT）作为模拟电子转移的框架。为了描述荧光光谱和动态斯托克斯位移，他们正在开发一种新的DFT和波函数技术的混合。 这些模拟是迄今为止对凝聚相光化学动力学最雄心勃勃的研究之一。这项研究正在开发一种通用的、广泛适用的技术，用于准确描述溶液中的光化学。 在这项研究过程中开发的技术适用于在光合作用，有机发光二极管（LED）和化学传感中发挥关键功能作用的分子。 世界各地的研究人员将通过Q-Chem一揽子计划获得这些方法，使潜在的影响基本上是无限的。研究生和博士后助理正在接受该项目的培训。PI和他的团队还根据他们的研究项目为普通观众制作基于网络的短片。 .

Troy Van Voorhis of the Massachusetts Institute of Technology is supported by an award from the Theory, Models and Computational Methods Program to develop, implement and apply transformative tools for modeling photochemical processes in complex environments. In particular, Van Voorhis and his research group focus on extending the techniques of ground state electronic structure theory to the accurate treatment of electronic excited states. They employ these new methods to understand three key photochemical processes: excited state intramolecular electron transfer (ET), ultrafast fluorescence spectroscopy and nonradiative quenching of dyes. They use constrained density functional theory (DFT) as a framework for simulating electron transfer. To describe fluorescence spectra and the dynamic Stokes shift they are developing a hybrid of novel DFT and wave function techniques. The simulations are among the most ambitious studies of condensed phase photochemical dynamics attempted to date.This research is developing a palette of general, widely applicable techniques for the accurate description of photochemistry in solution. The techniques developed in the course of this research are applicable to molecules that play key functional roles in photosynthesis, organic light-emitting diodes (LEDs) and chemical sensing. Researchers around the world will have access to these methods through the Q-Chem package of programs, making the potential impact essentially limitless. Graduate students and postdoctoral associates are being trained in this project. The PI and his group also produce, for a general audience, web-based short films based on their research projects. .