Plasmon-Driven Chemistry as Revealed by Ultrafast SERS, Single Molecule SERS, and Electrochemical TERS

超快 SERS、单分子 SERS 和电化学 TERS 揭示的等离激元驱动化学

• 批准号: 1807278
• 负责人: Michael Wasielewski
• 金额: $ 48万
• 依托单位: Northwestern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1807278&HistoricalAwards=false
• 关键词: Plasmon; Driven; Chemistry; Revealed; Ultrafast

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Van Duyne at Northwestern University is conducting studies to better understand how molecules behave and chemical reactions happen in the presence of a strong electromagnetic (EM) field induced by nearby plasmonic nanoparticles. Surface plasmon is a phenomenon from the oscillation of electrons on the surface of plasmonic nanoparticles collectively. Many factors affect how strong the EM field (i.e. the plasmonic field) is and how a molecule closely behaves. Professor Van Duyne plans to investigate the fundamental mechanisms of plasmon-driven chemistry, study the chemical enhancement contribution to single-molecule using a technique called surface-enhanced Raman spectroscopy (SM-SERS), and develop an electrochemical tip-enhanced Raman spectroscopy (EC-TERS) to interrogate how charge transfer across interfaces during chemical reactions. Fundamental insight gained from his study could enable new technological applications including photocatalysis, electrocatalysis, energy conversion and advance a wide array of technologies in multiple sectors including biosensing, defense, and healthcare. Professor Van Duyne works close with his graduate students and postdoctoral fellows, many women students, in his research group. He also plans to continue his outreach efforts to the public by hosting high school teachers in summers and interact with kids and their parents at an All Scout Nano Day on campus. Surface-enhanced femtosecond stimulated Raman spectroscopy (SE-FSRS) is applied to yield reaction mechanistic information across multiple time scales. In order to generalize single molecule surface-enhanced Raman spectroscopy to small molecules, chemical enhancement contribution is investigated to provide additional signal enhancement to boost the sensitivity of SMSERS. Professor Van Duyne plans to develop Electrochemical tip-enhanced Raman spectroscopy (EC-TERS) to elucidate the mechanisms of heterogeneous charge transfer reactions. EC-TERS can provide chemical information with spatial resolution down to the single site limit. Both fundamental understanding and novel applications of plasmonics on the nano and molecular scale is anticipated to be advanced through the proposed 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.

在化学系化学测量和成像计划的支持下，西北大学的Van Duyne教授正在进行研究，以更好地了解分子在附近等离子体纳米粒子诱导的强大电磁场(EM)存在下的行为和化学反应。表面等离子体激元是等离子体纳米粒子表面电子振荡的一种集体现象。许多因素影响电磁场(即等离子场)的强度以及分子行为的密切程度。Van Duyne教授计划研究等离子体激元驱动化学的基本机制，利用一种名为表面增强拉曼光谱(SM-SERS)的技术研究化学增强对单分子的贡献，并发展一种电化学尖端增强拉曼光谱(EC-TERS)来研究化学反应中电荷如何通过界面转移。从他的研究中获得的基本见解可以使新的技术应用成为可能，包括光催化、电催化、能源转换，并在生物传感、国防和医疗保健等多个领域推进广泛的技术。范·杜因教授在他的研究小组中与他的研究生和博士后研究员密切合作，其中许多是女性学生。他还计划继续向公众宣传，在暑假接待高中老师，并在校园里的全童子军纳米日与孩子和他们的父母互动。表面增强飞秒受激拉曼光谱(SE-FSRs)被用于获取多个时间尺度上的反应机理信息。为了将单分子表面增强拉曼光谱推广到小分子，研究了化学增强贡献，以提供额外的信号增强来提高SMSERS的灵敏度。Van Duyne教授计划发展电化学尖端增强拉曼光谱(EC-TERS)来阐明多相电荷转移反应的机理。EC可以提供精确到单站点极限的空间分辨率的化学信息。通过拟议的研究，预计将促进对纳米和分子尺度等离子体激元的基本理解和新的应用。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。

项目成果

Operando Characterization of Iron Phthalocyanine Deactivation during Oxygen Reduction Reaction Using Electrochemical Tip-Enhanced Raman Spectroscopy

• DOI: 10.1021/jacs.9b07979
• 发表时间: 2019-10-02
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Chen, Zhu;Jiang, Song;Van Duyne, Richard P.
• 通讯作者: Van Duyne, Richard P.

Plasmon-Driven Chemistry in Ferri-/Ferrocyanide Gold Nanoparticle Oligomers: A SERS Study

• DOI: 10.1021/jacs.0c05031
• 发表时间: 2020-07-29
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Qi, Yue;Brasiliense, Vitor;Van Duyne, Richard P.
• 通讯作者: Van Duyne, Richard P.