Probing Molecular Dynamics Near Plasmonic Surfaces by Optical two-dimensional Coherent Spectroscopy

通过光学二维相干光谱探测等离子体表面附近的分子动力学

• 批准号: 2003785
• 负责人: Hebin Li
• 金额: $ 45万
• 依托单位: Florida International University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2003785&HistoricalAwards=false
• 关键词: Probing; Molecular; Dynamics; Near; Plasmonic

With this award, the Chemical Measurement and Imaging Program in the Chemistry Division, with co-funding from the Atomic, Molecular and Optical Physics - Experiment Program in the Physics Division, is funding Drs. Hebin Li and Jin He at Florida International University (FIU) to develop a novel integrated ultrafast spectroscopy and imaging technique for studying molecular dynamics. The ability to probe ultrafast chemical behavior of molecules and electrons at the nanometer scale is essential for studying and understanding materials, such as deoxyribonucleic acid (DNA) molecules, proteins linked to photosynthesis, novel solar cell layers, and exotic quantum materials. Advanced laser spectroscopy, such as optical two-dimensional coherent spectroscopy (2DCS), excels in studying chemical behavior in complex systems, while the spatial resolution is usually limited to the millionth of meter scale. On the other hand, the scanning tunneling microscope (STM) provides nanometer resolution for single-molecule studies, while the measurements in STM are limited to the millisecond timescale. Drs. Hebin Li and Jin He and their research team integrate optical 2DCS and STM-based single-molecule techniques to acquire chemical information about surfaces with nanometer resolution spatial mapping and femtosecond time resolution. The novel imaging technique enables understanding and improving numerous chemical and materials systems. By engaging students in active research and connecting to local science teachers, the project also makes an important contribution to the goal of FIU, a minority-serving institution, to strengthen the education of underrepresented groups in science, technology, engineering, and mathematics (STEM) fields, and to promote public interest in science in South Florida.The primary goal of this project is to develop surface-enhanced optical two-dimensional coherent spectroscopy (2DCS) to probe molecular dynamics on plasmonic surfaces by implementing optical 2DCS on a metal nanoelectrode (NE) to achieve a high spatial resolution. The developed technique has integrated advantages of both STM and optical 2DCS, including high spatial resolution, high detection sensitivity, femtosecond temporal resolution, and multidimensional capability. Using this technique to study molecules on the metal NE surface and molecular junctions in the nanogap between two metal nanostructures, the research enables new capabilities to probe charge transfer dynamics at molecule-metal and molecule-molecule interfaces, intermolecular interactions in small molecule pairs, and the dynamics of hydrogen-bonding patterns and networks in proteins at metal-molecule-metal junctions. The unique capabilities of this approach can potentially lead to novel applications in studying other systems such as two-dimensional and perovskite materials, photosynthetic proteins, and biological molecules.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.

凭借该奖项，化学部的化学测量和成像项目，在物理部原子、分子和光学物理 - 实验项目的共同资助下，正在资助 Drs.佛罗里达国际大学 (FIU) 的 Hebin Li 和 Jin He 开发了一种用于研究分子动力学的新型集成超快光谱和成像技术。在纳米尺度上探测分子和电子的超快化学行为对于研究和理解材料至关重要，例如脱氧核糖核酸 (DNA) 分子、与光合作用相关的蛋白质、新型太阳能电池层和奇异的量子材料。先进的激光光谱，例如光学二维相干光谱（2DCS），擅长研究复杂系统中的化学行为，但空间分辨率通常仅限于百万分之一米尺度。另一方面，扫描隧道显微镜 (STM) 为单分子研究提供纳米分辨率，而 STM 的测量仅限于毫秒时间尺度。博士。 Hebin Li 和 Jin He 及其研究团队集成了光学 2DCS 和基于 STM 的单分子技术，以纳米分辨率空间映射和飞秒时间分辨率获取表面化学信息。新颖的成像技术能够理解和改进众多化学和材料系统。 通过让学生积极参与研究并与当地科学教师建立联系，该项目还为佛罗里达国际大学（一家为少数族裔服务的机构）的目标做出了重要贡献，即加强对科学、技术、工程和数学领域代表性不足群体的教育（STEM ）领域，并促进南佛罗里达州公众对科学的兴趣。该项目的主要目标是开发表面增强光学二维相干光谱（2DCS），通过在金属纳米电极上实施光学 2DCS 来探测等离子体表面的分子动力学（NE）以实现高空间分辨率。该技术综合了STM和光学2DCS的优点，包括高空间分辨率、高检测灵敏度、飞秒时间分辨率和多维能力。利用该技术研究金属 NE 表面上的分子和两个金属纳米结构之间纳米间隙中的分子连接，该研究能够探测分子-金属和分子-分子界面上的电荷转移动力学、小分子对中的分子间相互作用以及金属-分子-金属连接处蛋白质中氢键模式和网络的动力学。这种方法的独特功能可能会在研究其他系统（例如二维和钙钛矿材料、光合蛋白质和生物分子）方面带来新的应用。该奖项反映了 NSF 的法定使命，并通过使用基金会的评估进行评估，被认为值得支持。智力价值和更广泛的影响审查标准。

项目成果

Probing the Intermediates of Catalyzed Dehydration Reactions of Primary Amide to Nitrile in Plasmonic Junctions

等离子体连接中伯酰胺催化脱水反应中间体的探讨

• DOI: 10.1021/acscatal.2c01793
• 发表时间: 2022-06-14
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Jianghao Zhou;Jing Guo;A. Mebel;Govinda Ghimire;Feng Liang;Shuai Chang;Jin He
• 通讯作者: Jin He

Reversibly Modulating Plasmon‐mediated Chemical Reaction via Electrode Potential on Reliable Copper Nanoelectrode

通过可靠的铜纳米电极上的电极电势可逆地调节等离子体介导的化学反应

• DOI: 10.1002/anie.202302215
• 发表时间: 2023-04
• 期刊: Angewandte Chemie International Edition
• 作者: Ghimire, Govinda;Guo, Jing;Halmagian, Robert;He, Jin
• 通讯作者: He, Jin

Potentiometric and SERS Detection of Single Nanoparticle Collision Events on a Surface Functionalized Gold Nanoelectrode

表面功能化金纳米电极上单纳米粒子碰撞事件的电位和 SERS 检测

• DOI: 10.1149/1945-7111/ac6245
• 发表时间: 2022-04
• 期刊: Journal of The Electrochemical Society
• 影响因子: 3.9
• 作者: Ghimire, Govinda;Pandey, Popular;Guo, Jing;Sarker, Golam Sabbir;Moon, Joong Ho;He, Jin
• 通讯作者: He, Jin

Broadband optical two-dimensional coherent spectroscopy of a rubidium atomic vapor

铷原子蒸气的宽带光学二维相干光谱

• DOI: 10.1103/physreva.105.052810
• 发表时间: 2022-05
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Yan, Jieli;Revesz, Stephen;Liang, Danfu;Li, Hebin
• 通讯作者: Li, Hebin

Direct Observation of Amide Bond Formation in a Plasmonic Nanocavity Triggered by Single Nanoparticle Collisions

直接观察单纳米粒子碰撞引发的等离激元纳米腔中酰胺键的形成

• DOI: 10.1021/jacs.1c02426
• 发表时间: 2021-07
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Kong, Na;Guo, Jing;Chang, Shuai;Pan, Jie;Wang, Jianmei;Zhou, Jianghao;Liu, Jing;Zhou, Hong;Pfeffer, Frederick M.;Liu, Jingquan;et al
• 通讯作者: et al