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.

在得克萨斯大学圣安东尼奥分校化学系的化学结构，动力学和机制-B（CSDM-B）计划的支持下，北佐治亚大学化学系的化学学院化学系的Kirk S. Schanze教授以及北乔治大学化学系的AiméeTomlinson教授正在研究带有收费的有机化物质的物业的物业，这些物质是有用的。该项目位于有机，物理和计算化学的界面，非常适合各个级别的化学科学家进行广泛的教育。调查人员将利用各自大学的潜水员人群在研究的各个方面让代表性不足的学生与人数不足。这项合作将为参与的研究学生访问理论和实验之间的反馈回路，从而丰富其化学研究项目。本项目旨在通过涉及实验性摄影和计算化学方法，使用密度函数理论和依赖性密度的密度函数理论来控制控制离子自由基激发态及其电子传输反应的因素。各种分子的稳定阴离子和阳离子自由基将通过化学还原或氧化，然后通过皮秒瞬间滥用和荧光光谱法表征其光物理特性。要确定的关键参数包括双线激发态的寿命和能量，以及辐射和非辐射衰减速率常数。实验结果将用于为离子自由基双重激发态的结构 - 特性关系提供信息，具体目的是描述能量差异和非辐射性衰减率之间是否存在能量差距法相关性。理论将用于识别针对双重激发态能量和生命周期进行优化的分子系统，从而指导设计优化的电子传输光感增强剂的设计。该奖项反映了NSF的法定任务，并被认为是通过基金会的知识分子和更广泛影响的评估标准通过评估来评估的。