Pure Electronic Rydberg Spectroscopy: The Use of Chirped-Pulse Millimeter-Wave and Time-Domain TeraHertz Spectroscopies to Reveal the Mechanisms of Electron<-->Cation

纯电子里德伯光谱：使用啁啾脉冲毫米波和时域太赫兹光谱揭示电子机制

• 批准号: 0749821
• 负责人: Robert Field
• 金额: $ 75.4万
• 依托单位: Massachusetts Institute of Technology
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2008
• 资助国家: 美国
• 起止时间: 2008-02-15 至 2012-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0749821&HistoricalAwards=false
• 关键词: Pure; Electronic; Rydberg; Spectroscopy; Use

Robert Field of MIT is supported by the Experimental Physical Chemistry Program to develop experimental methods, theoretical models, and intuitive concepts by which the mechanisms for exchange of energy and angular momentum between an electron and a molecular cation may be characterized. Experiments will be carried out on small, gas phase molecules in highly excited electronic states with the goal of generating fundamental insights into the mechanisms and strength of its electron - nuclear coupling that are germane to larger molecules, at all excitation energies, and in condensed phases. Chirped-pulse millimeter-wave spectroscopy will be used in combination with multiple nanosecond dye laser excitation, in multi-laser schemes that will enable the probing of molecular Rydberg launch states under supersonic molecular beam conditions. Pure electronic spectroscopy studies of molecules of increasing spectroscopic and dynamical complexity (CaF, CaCl, and nitrogen dioxide) are expected to demonstrate the power of the combined nanosecond tunable laser/Chirped-pulse millimeter-wave approaches to characterize, with a minimum of spectroscopic detective work, important electron - nuclear energy exchange mechanisms including their dependence on molecular geometries.Electron transport, electronic energy harvesting and disposal, and the making and breaking of chemical bonds all involve the exchange of energy between electrons and nuclei in molecules. Research outcomes from this effort have the potential to lead to important impacts in the understanding of energy couplings and flow in molecules. This project will enable effective research training of students. As well, Field has written an expanded and refocused textbook in molecular spectroscopy that is expected to be valuable for research and education applications.

麻省理工学院的罗伯特·菲尔德在实验物理化学项目的支持下开发实验方法、理论模型和直观概念，通过这些概念可以表征电子和分子阳离子之间能量和角动量交换的机制。实验将在处于高度激发电子态的小气相分子上进行，目的是对其电子-核耦合的机制和强度产生基本的了解，这些耦合与较大分子、在所有激发能量下和在凝聚相中密切相关。 。 啁啾脉冲毫米波光谱将与多纳秒染料激光激发结合使用，在多激光方案中，这将能够在超音速分子束条件下探测分子里德伯发射态。对光谱和动力学复杂性不断增加的分子（CaF、CaCl和二氧化氮）进行纯电子光谱研究预计将证明纳秒可调谐激光/啁啾脉冲毫米波方法相结合的能力，以最少的光谱检测来表征工作，重要的电子-核能量交换机制，包括它们对分子几何形状的依赖。电子传输、电子能量收集和处理，以及化学键的形成和断裂都涉及电子和原子核之间的能量交换在分子中。这项工作的研究成果有可能对理解分子中的能量耦合和流动产生重要影响。该项目将为学生提供有效的研究培训。此外，菲尔德还撰写了一本扩展并重新调整重点的分子光谱学教科书，预计对研究和教育应用有价值。