Collaborative Research: Ultrafast Excited State Electron and Nuclear Coherences in Transition Metal Dimer Complexes and Their Roles in Photochemistry

合作研究：过渡金属二聚体配合物中的超快激发态电子和核相干性及其在光化学中的作用

基本信息

批准号：
1665021
负责人：
Lin Chen
金额：
$ 27.5万
依托单位：
Northwestern University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-08-01 至 2020-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1665021&HistoricalAwards=false
关键词：
Collaborative Research Ultrafast Excited State

项目摘要

In this project funded by the Chemical Structure, Dynamic & Mechanism B Program of the Chemistry Division, Professors Lin X. Chen and Felix N. Castellano are developing the spectroscopy and chemistry necessary for the study of transition metal complexes featuring dimetallic cooperativity. These targeted molecules convert and accumulate energy from sunlight that can ultimately drive photocatalytic reactions for generating fuels. The knowledge obtained through these studies could be transformative for the chemical sciences and will enhance our ability to rationally design chemical materials/devices for catalysis, optoelectronics and energy sustainability. The research engages university graduate students to use advanced laser spectroscopy for characterization, incorporates state-of-the-art computational chemistry for quantum mechanical and molecular dynamics modeling, and utilizes advanced chemistry laboratory facilities for molecular synthesis, providing them with an expansive training ground for the development of multidisciplinary expertise. Such training is urgently needed for the next generation STEM workforce in order to explore the frontiers of chemical science and to ensure US global competitiveness at the frontiers of scientific knowledge.The work studies quantum coherence in a series of di-metallic compounds, such as platinum, molybdenum, and tungsten dimer chromophores through systematic variation of structural factors. Mechanistic details enabling multiple-electron conversion processes are to be investigated through two-dimensional electronic spectroscopy and by the design of new molecular architectures. The research seeks an understanding of intrinsic electronic couplings between multiple metal centers in transition metal complexes and their influence on photochemical reactivity. Using ultrafast laser pulses as light sources, transient bond-making or bond-breaking processes will be induced between the two metal centers, which enable detailed studies on origins of their catalytic activities and fundamental reaction dynamics.

在化学结构，动态和机制B计划资助的该项目中，林克·陈（Lin X.这些靶向分子从阳光转化并积累了能量，最终可以驱动光催化反应以产生燃料。通过这些研究获得的知识可能是化学科学的变革性，并将增强我们合理设计化学材料/设备用于催化，光电和能量可持续性的能力。这项研究与大学研究生一起使用先进的激光光谱进行表征，并结合了量子机械和分子动力学建模的最先进的计算化学，并利用了高级化学实验室设施进行分子合成，为他们提供了广泛的训练场，以开发多学科专业知识。下一代STEM劳动力迫切需要进行这种训练，以探索化学科学的前沿并确保我们在科学知识的边界上进行全球竞争力。研究研究在一系列双金属化合物中的量子相干性，例如铂，钼，以及通过结构性变量的二型二聚体粒子。可以通过二维电子光谱和新分子体系结构的设计来研究实现多电子转换过程的机械细节。该研究寻求了解过渡金属复合物中多个金属中心之间的内在电子耦合及其对光化学反应性的影响。将使用超快激光脉冲作为光源，将在两个金属中心之间诱发瞬态键合或断开键的过程，这可以详细研究其催化活性的起源和基本反应动力学。