CAREER: Development of Single Molecule Infrared and Visible Absorption Spectroscopies using Optical Trapping Force Detection

职业：利用光学捕获力检测开发单分子红外和可见吸收光谱

• 批准号: 1752847
• 负责人: Ziad Ganim
• 金额: $ 62.44万
• 依托单位: Yale 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: 2018-07-01 至 2022-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1752847&HistoricalAwards=false
• 关键词: CAREER; Development; Single; Molecule; Infrared

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Ganim at Yale University is building microscopes that combine sensitivity (down to one molecule) with broad compatibility (any molecule, any solvent environment, bio/non-biological reactivity, etc.) and produce straightforward spectral data that any chemist can interpret. Professor Ganim uses a combination of ultrafast infrared spectroscopy with precision force microscopy to help scientists to watch the distribution of intermediates occurring in a chemical reaction one at a time. The results could provide new experimental and theoretical insights to comprehensively quantify distributions of molecular structures that naturally occur. Professor Ganim also works with three educational initiatives on campus. Exemplary projects include interactive demonstrations for students to pull and push at the microscopic world using a research-grade optical trap and workshops to build and take home a functional spectrometer and microscope.The support project is motivated by the transformative progress that will be possible when measuring reaction kinetics in complex mixtures is simple enough that chemists will apply it to study the mechanisms of failed reactions. Professor Ganim builds on the recent development of force-detected nanoscale absorption spectroscopy in solution and develops single molecule (SM) infrared spectroscopy suitable for chemical kinetics experiments. Specifically Professor Ganim and his group develop a predictive model to explain the photoinduced signal magnitude and to guide the synthesis of custom nanostructured force probes. Traditional SM fluorescence is used to independently verify single molecule sensitivity. These enhancements are then used in conjunction with a multiplexed, time-domain implementation and maximum-likelihood signal processing to realize SM infrared spectroscopy. The technique is then used to observe real-time ligand exchange in single iridium(III) hydride complexes, which are known for their catalytic hydrogenation and dehydrogenation properties.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项目的支持下，耶鲁大学的Ganim教授正在建造将联合收割机灵敏度（低至一个分子）与广泛兼容性（任何分子，任何溶剂环境，生物/非生物反应性等）相结合的显微镜。并产生任何化学家都能解释的简单光谱数据。Ganim教授使用超快红外光谱与精密力显微镜相结合，帮助科学家一次一个地观察化学反应中发生的中间产物的分布。这些结果可以为全面量化自然发生的分子结构分布提供新的实验和理论见解。 Ganim教授还在校园内开展三项教育活动。示范项目包括互动演示，让学生使用研究级光阱在微观世界中推拉，以及制作并带回家功能光谱仪和显微镜的研讨会。支持项目的动机是，当测量复杂混合物中的反应动力学足够简单时，化学家将其应用于研究失败反应的机制时，将有可能实现变革性的进步。Ganim教授基于最近在溶液中力检测纳米吸收光谱的发展，开发了适用于化学动力学实验的单分子（SM）红外光谱。 具体来说，Ganim教授和他的团队开发了一个预测模型来解释光诱导信号的大小，并指导定制纳米结构力探针的合成。传统的SM荧光用于独立验证单分子灵敏度。这些增强，然后结合使用的多路复用，时域实现和最大似然信号处理，实现SM红外光谱。该技术被用于观察单个铱（III）氢化物络合物中的实时配体交换，该络合物以其催化氢化和脱氢性能而闻名。该奖项反映了NSF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而被认为值得支持。