Improved Methods for Including Vibronic and Environmental Effects in Simulations of Optical Spectroscopy

加州大学默塞德的克莉丝汀·伊斯伯恩教授获得了化学系化学理论、模型和计算方法项目的一项奖励，以开发和应用模拟光谱学的改进方法。 她的研究重点是发色团（光吸收剂）周围的环境（例如溶剂，表面，蛋白质）如何影响电子激发态。将开发新的模拟技术，更好地代表原子和实验细节。模拟复杂环境中的光谱学的新方法可以用来指导具有所需光学特性的新分子和材料的设计。改进的光学光谱模拟工具将提高对复杂环境中电子激发过程的理解，并有可能推动光化学、电光或光催化领域的新技术。 教授Isborn还从事在高中，本科和研究生水平更广泛的影响活动。为了服务主要是第一代学生群体，本科生用英语和学生的母语创作短视频，讨论他们的经历。为期一周的研究生水平暑期学校侧重于计算机理论的基础和应用，有助于培养下一代化学家的未来劳动力。光谱学，包括光吸收、荧光和时间分辨超快电子光谱学，是探测许多化学系统和分子反应的电子行为的最常用技术。这些方法对环境影响敏感，然而，用于在复杂环境中对分子的光谱进行建模的传统方法通常由于缺乏振动效应和/或缺少分子与其环境之间的特定相互作用而无法再现光谱形状。Isborn教授和她的团队正在开发一系列用于模拟光学吸收，荧光和超快光谱的方法，这些方法通过计算原子环境中存在的基础和激发振动模式来解释振动跃迁和特定的溶质-溶剂-环境相互作用。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Professor Christine Isborn of the University of California Merced is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop and apply improved methods for simulating optical spectroscopy. Her research focuses on how the environment (e.g. solvent, surface, protein) surrounding a chromophore (light absorber) affects the electronic excited states. New simulation techniques will be developed that better represent atomistic and experimental details.The new methods for simulating optical spectroscopy in complex environments can be used to guide the design of new molecules and materials that have desired optical properties. Improved tools for simulating optical spectroscopy will improve understanding of electronic excitation processes in complex environments, with the potential for this increased understanding to drive new technologies in the fields of photovoltaics, electro-optics, or photo-catalysis. Professor Isborn also engages in broader impact activities at the high school, undergraduate, and graduate student levels. To serve a primarily first-generation student population, undergraduate students create short videos in both English and the student’s native language in which they discuss their experiences. A week-long graduate student level summer school focused on the fundamentals and applications of computer theory helps to train the next generation of chemists for the workforce of the future. Optical spectroscopy, including optical absorption, fluorescence, and time-resolved ultrafast electronic spectroscopy, is the most commonly used technique for probing the electronic behavior of many chemical systems and molecular reactions. These methods are sensitive to environmental effects, however, traditional approaches for modeling optical spectra of molecules in complex environments often fail to reproduce spectral shapes due to either lacking vibronic effects and/or missing specific interactions between the molecule and its environment. Professor Isborn and her group are developing a family of approaches for simulating optical absorption, fluorescence, and ultrafast spectra that account for both vibronic transitions and specific solute-solvent-environment interactions by computing ground and excited vibrational modes in the presence of the atomistic environment. They are examining how the environment affects spectral shapes and electronic relaxation for a variety of chromophores within complex environments.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.