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·菲尔德得到了实验物理化学计划的支持，以开发实验方法，理论模型和直观的概念，通过这些概念可以表征电子和分子阳离子之间的能量和角动量交换机制。实验将在高激发电子态的小气相分子上进行，目的是在所有激发能量下和凝聚相中产生对其电子-核耦合机制和强度的基本见解，这些机制和强度与较大分子密切相关。 啁啾脉冲毫米波光谱学将与多纳秒染料激光激发相结合，在多激光方案中，将使分子里德伯发射状态在超音速分子束条件下的探测成为可能。光谱和动力学复杂性增加的分子的纯电子光谱研究（CaF、CaCl和二氧化氮）的实验结果表明，纳秒可调谐激光器/啁啾脉冲毫米波组合方法能够以最少的光谱探测工作表征重要的电子-核能交换机制，包括它们对分子几何形状的依赖性。电子能量的收集和处理以及化学键的形成和断开都涉及分子中电子和原子核之间的能量交换。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。该项目将使学生能够进行有效的研究培训。此外，菲尔德还写了一本扩展和重新聚焦的分子光谱学教科书，预计对研究和教育应用有价值。