CAREER: Investigating Ultrafast Electronic and Structural Dynamics During Light-Driven Chemical Reactions

职业：研究光驱动化学反应期间的超快电子和结构动力学

• 批准号: 1753324
• 负责人: Daniel Rolles
• 金额: $ 50万
• 依托单位: Kansas State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-08-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1753324&HistoricalAwards=false
• 关键词: CAREER; Investigating; Ultrafast; Electronic; Structural

This project will develop new experimental tools for imaging ultrafast dynamics during photochemical reactions in molecules. This will enable new studies of light-induced reactions that are important in several scientific areas. For example, photochemical dissociation reactions play a major role in atmospheric chemistry. Light-induced molecular ring-opening and isomerization reactions also serve as prototypes for understanding biosynthesis of vitamin D, controlling the dynamics of organic molecular switches, and engineering novel light-harvesting materials. Imaging and controlling such reactions at the electronic level can therefore lead to the development of new technologies with potential benefits to society. This project will engage students from diverse backgrounds and foster their interest in basic science and technology disciplines by introducing them early in their academic career to scientific research. Students will benefit from a variety of research environments ranging from a state-of-the-art laser laboratory at a university to large-scale user facilities operated at national laboratories.To further the understanding of the ultrafast electronic and structural dynamics occurring during light-driven reactions, this project will use femtosecond light sources combined with powerful detection techniques such as coincident electron and ion momentum imaging and time-resolved photoelectron spectroscopy. These tools will be used to study isomerization and ring-opening reactions in organic molecules with chemical relevance. Femtosecond pump-probe techniques with laboratory-based femtosecond lasers and high-order harmonic generation sources will be complemented by experiments with free-electron lasers. Being able to record "molecular movies" of benchmark photochemical reactions will allow for a more direct comparison to quantum chemistry calculations. The aim is to provide a better understanding of the underlying reaction mechanism and to develop and optimize schemes for controlling the dynamics and outcome of such reactions.This project is jointly funded by the Atomic, Molecular, and Optical Physics Experiment program in the Division of Physics and the Chemical Measurement and Imaging program in the Division of Chemistry (both Divisions are in the NSF Directorate for Mathematical and Physical Sciences) as well as the Established Program to Stimulate Competitive Research.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.

本项目将开发新的实验工具，用于成像分子光化学反应过程中的超快动力学。这将使光诱导反应的新研究成为可能，这在几个科学领域都很重要。例如，光化学解离反应在大气化学中起着重要作用。光诱导的分子开环和异构化反应也可以作为理解维生素D生物合成、控制有机分子开关动力学和设计新型光收集材料的原型。因此，在电子水平上对这种反应进行成像和控制可以导致新技术的发展，对社会有潜在的好处。该项目将吸引来自不同背景的学生，通过在他们的学术生涯早期将他们引入科学研究，培养他们对基础科学和技术学科的兴趣。学生将受益于各种研究环境，从大学最先进的激光实验室到国家实验室运行的大型用户设施。为了进一步了解在光驱动反应中发生的超快电子和结构动力学，该项目将使用飞秒光源结合强大的检测技术，如同步电子和离子动量成像和时间分辨光电子能谱。这些工具将用于研究具有化学相关性的有机分子中的异构化和开环反应。利用实验室飞秒激光器和高次谐波源的飞秒泵浦探测技术将被自由电子激光器的实验所补充。能够记录基准光化学反应的“分子电影”将允许与量子化学计算进行更直接的比较。目的是更好地了解潜在的反应机制，并制定和优化控制这种反应的动力学和结果的方案。该项目由物理系的原子、分子和光学物理实验项目和化学系的化学测量和成像项目（这两个部门都隶属于NSF数学和物理科学理事会）以及促进竞争性研究的既定计划共同资助。该奖项反映了美国国家科学基金会的法定使命，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。

项目成果

Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy

使用超快 XUV-Vis 泵浦探针光谱法探索芴的裂解动力学

• DOI: 10.3389/fphy.2022.880793
• 发表时间: 2022
• 期刊: Frontiers in Physics
• 影响因子: 3.1
• 作者: Garg, D.;Lee, J. W.;Tikhonov, D. S.;Chopra, P.;Steber, A. L.;Lemmens, A. K.;Erk, B.;Allum, F.;Boll, R.;Cheng, X.
• 通讯作者: Cheng, X.

Two- and three-body fragmentation of multiply charged tribromomethane by ultrafast laser pulses

• DOI: 10.1039/d2cp03089f
• 发表时间: 2022-10-27
• 期刊: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
• 影响因子: 3.3
• 作者: Bhattacharyya, Surjendu;Borne, Kurtis;Rolles, Daniel
• 通讯作者: Rolles, Daniel

High harmonic generation in mixed XUV and NIR fields at a free-electron laser

自由电子激光器在 XUV 和 NIR 混合场中产生高次谐波

• DOI: 10.1088/2040-8986/ac4318
• 发表时间: 2022
• 期刊: Journal of Optics
• 影响因子: 2.1
• 作者: Troß, Jan;Pathak, Shashank;Summers, Adam;Rompotis, Dimitrios;Erk, Benjamin;Passow, Christopher;Manschwetus, Bastian;Boll, Rebecca;Grychtol, Patrik;Bari, Sadia
• 通讯作者: Bari, Sadia