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.

该项目将开发新的实验工具，用于在分子中的光化学反应期间成像超快动力学。这将使在几个科学领域很重要的光引起的反应进行新的研究。 例如，光化学解离反应在大气化学中起主要作用。 光诱导的分子环和异构化反应也是理解维生素D的生物合成，控制有机分子开关的动力学以及工程新型的轻度收获材​​料的原型。因此，在电子水平上进行成像和控制这种反应可以导致发展具有潜在利益的新技术。该项目将吸引来自不同背景的学生，并通过将学术职业的早期引入科学研究来培养他们对基础科学和技术学科的兴趣。 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光谱法。 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。 使用基于实验室的飞秒激光器和高阶谐波生成来源的飞秒泵探针技术将通过自由电子激光器进行补充。能够记录基准光化学反应的“分子电影”将与量子化学计算进行更直接的比较。 其目的是为了更好地理解潜在的反应机制，并制定和优化方案来控制此类反应的动态和结果。该项目由物理学划分的原子，分子和光学物理实验计划共同资助。刺激竞争性研究。该奖项反映了NSF的法定使命，并被认为是值得通过基金会的知识分子优点和更广泛影响的评论标准来评估值得支持的。

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