CAS: Collaborative Research: Photophysics and Electron Transfer Reactivity of Ion Radical Excited States

CAS：合作研究：离子自由基激发态的光物理学和电子转移反应性

• 批准号: 2246509
• 负责人: Aimee Tomlinson
• 金额: $ 17.86万
• 依托单位: University of North Georgia
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-06-01 至 2026-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2246509&HistoricalAwards=false
• 关键词: CAS; Collaborative; Research; Photophysics; Electron

With support of the Chemical Structure, Dynamics & Mechanisms-B (CSDM-B) Program of the Chemistry Division, Professor Kirk S. Schanze of the Department of Chemistry at the University of Texas at San Antonio, and Professor Aimée Tomlinson of the Department of Chemistry at the University of North Georgia are studying the properties of charged organic radicals with useful properties as photosensitizers for organic reactions and solar energy conversion. The project lies at the interface of organic, physical, and computational chemistry and is well suited for broad education of chemical scientists at all levels. The investigators will leverage the diverse populations at their respective universities to engage underrepresented students in all aspects of the research. This collaboration will provide engaged research students access to the feedback loop between theory and experiment thus enriching their chemical research projects.This project seeks to provide an understanding of the factors that control ion radical doublet excited states and their electron transfer reactivity, through a collaborative approach involving experimental photophysics and computational chemistry using density functional theory and time dependent density functional theory. Stable anion and cation radicals of a variety of molecules will be prepared by chemical reduction or oxidation followed by characterization of their photophysical properties through picosecond transient absorption and fluorescence spectroscopy methods. Key parameters to be determined include the lifetime and energy of the doublet excited state, along with the radiative and non-radiative decay rate constants. The experimental results will be utilized to inform structure-property relationships for the ion radical doublet excited states, with specific aim to delineate whether an energy gap law correlation exists between their energy and non-radiative decay rate. Theory will be used to identify molecular systems that are optimized with respect to doublet excited state energy and lifetime thereby, guiding the design of optimized electron transfer photosensitizers.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.

在化学部化学结构、动力学与机理-B（CSDM-B）项目的支持下，德克萨斯大学圣安东尼奥分校化学系Kirk S. Schanze教授和化学系Aimée Tomlinson教授北乔治亚大学的化学系正在研究带电有机自由基的特性，这些自由基具有作为有机反应和太阳能转换的光敏剂的有用特性，该项目位于有机、物理和计算化学与有机化学的交叉领域。非常适合各个级别的化学科学家的广泛教育。研究人员将利用各自大学的不同人群，让代表性不足的学生参与研究的各个方面。这种合作将为参与研究的学生提供理论与研究之间的反馈循环。实验，从而丰富了他们的化学研究项目。该项目旨在通过使用密度泛函理论和时间相关密度泛函的涉及实验光物理学和计算化学的协作方法，提供对控制离子自由基双激发态及其电子转移反应性的因素的理解稳定的阴离子和各种分子的阳离子自由基将通过化学还原或氧化来制备，然后通过皮秒瞬态吸收和荧光光谱方法表征其光物理性质，待确定的关键参数包括双激发态的寿命和能量，以及实验结果将用于了解离子自由基双激发态的结构-性质关系，具体目的是描述它们的能量和能量之间是否存在能隙定律相关性。理论将用于识别在双态激发态能量和寿命方面优化的分子系统，指导优化电子转移光敏剂的设计。该奖项的法定使命，并通过评估被认为值得支持。利用基金会的智力优势和更广泛的影响审查标准。