Ultrafast Dynamics Occurring in the Ground States of Transition Metal Ccmplexes

过渡金属复合物基态中发生的超快动力学

• 批准号: 2153757
• 负责人: Clifford Kubiak
• 金额: $ 54.5万
• 依托单位: University of California-San Diego
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-08-01 至 2025-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2153757&HistoricalAwards=false
• 关键词: Ultrafast; Dynamics; Occurring; Ground; States

In this project, funded by the Chemical Structure, Dynamics, and Mechanisms B Program of the Chemistry Division, Professor Clifford Kubiak of the Department of Chemistry and Biochemistry at the University of California San Diego is developing new assemblies of metal complexes that undergo fast electron transfer (ET) reactions. Electron transfer (ET) is the basis of operation of every electronic device. ET research can elucidate methods for efficient conversion of light to electrons and, subsequently, usable and storable chemical energy. This NSF-funded project investigates a new generation of mixed-valent complexes to study the behavior of electronic delocalization in molecular systems. The ramifications of these findings can extend to the development of integrated circuits, quantum computing, and artificial photosynthesis. In tandem with this project, Professor Kubiak’s group is also dedicated to community outreach and science education, engaging and involving K-12 and undergraduate students in cutting edge fundamental science.Mixed-valent trinuclear oxo-bridged clusters have proven to be valuable model systems for the development and understanding of the factors that control the rates, switching location, and polarization of ground state electron transfer on the ultrafast (picosecond) timescale using infrared spectroscopy and electrochemistry to probe these phenomena. The most recent support period informed several key aims for future research, including: (i) covalent attachment of mixed-valent complexes to electrode surfaces and measurement of the influence of electric fields on mixed-valent complexes potential energy surfaces; (ii) extending the study of electric field driven ET towards driving chemical reactions important to catalysis; (iii) the study of mixed-valent complexes joined by chiral bridges to understand interactions between chiral molecules and spin; and (iv) the preparation and study of high-spin mixed-valent iron clusters.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.

在这个由化学系化学结构、动力学和机制B计划资助的项目中，加州大学圣地亚哥分校化学和生物化学系的Clifford Kubiak教授正在开发经历快速电子转移(ET)反应的金属络合物的新组件。电子转移是每一种电子设备运行的基础。ET研究可以阐明有效地将光转化为电子的方法，以及随后可用和可储存的化学能。这项由美国国家科学基金会资助的项目研究了新一代混价络合物，以研究分子体系中的电子离域行为。这些发现的结果可以延伸到集成电路、量子计算和人工光合作用的发展。在这个项目的同时，库比亚克教授的团队还致力于社区推广和科学教育，让K-12和本科生参与尖端基础科学。混合价三核氧桥簇已被证明是有价值的模型系统，用于开发和理解控制超快(皮秒)时间尺度上基态电子转移的速率、开关位置和极化的因素，使用红外光谱和电化学来探索这些现象。最近的支撑期揭示了未来研究的几个关键目标，包括：(I)混价络合物与电极表面的共价连接以及电场对混价络合物势能面的影响；(Ii)将电场驱动电子转移的研究扩展到驱动对催化重要的化学反应；(Iii)通过手性桥连接的混价络合物的研究，以了解手性分子与自旋之间的相互作用；以及(Iv)高自旋混合价铁簇合物的准备和研究。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。