High Resolution Spectroscopy of Reactive Chemical Intermediates and Related Studies

美国俄亥俄州立大学的Terry a . Miller教授及其课题组将利用高分辨率空腔衰荡光谱（HR-CRDS）技术，获取并分析与对流层化学相关的多种活性化学中间体的光谱，包括有机过氧自由基、硝酸盐自由基和羟基烷氧自由基。米勒实验室开发的一项名为远红外/中红外共振增强多光子电离双共振光谱（FIR/MIR-REMPI-DRS）的新技术将用于将光谱研究扩展到更长的波长，并获得碳链（与天体化学相关）和生物相关分子（如氨基酸）等物种的高分辨率光谱。这些研究将为自由基和其他在燃烧和大气化学中重要的分子提供诊断标记，并将高分辨率光谱扩展到可以提供大分子特征信息的光谱低频区域。光谱分析也将提供精确的分子参数，可以作为实验？黄金标准?指导和基准电子结构计算。拟议研究的更广泛的科学影响包括与对流层化学、天体化学和生物化学相关的有价值的光谱数据和诊断。此外，从事这些项目的年轻研究人员将获得物理化学方面的良好培训——在复杂的实验和理论方法方面获得宝贵的经验。米勒教授将继续开发以研究为基础的研究生课程，强调分子光谱学的广泛应用，并开发一个适合化学入门课程的相同主题的新模块。

In this project supported by the Chemical Structure, Dynamics and Mechanisms Program of the Chemistry Division, Prof. Terry A. Miller of Ohio State University and his research group will utilize high resolution cavity ring-down spectroscopy (HR-CRDS) to obtain and analyze the spectra of a number of reactive chemical intermediates relevant to tropospheric chemistry, including organic peroxy radicals, nitrate radicals, and hydroxy alkoxy radicals. A new technique developed in the Miller laboratory called far-infrared/mid-infrared resonance enhanced multiphoton ionization double-resonance spectroscopy (FIR/MIR-REMPI-DRS) will be used to extend spectral studies to longer wavelengths and obtain high resolution spectra of species like carbon chains (relevant to astrochemistry) and biologically relevant molecules such as amino acids. These studies will provide diagnostic markers for radicals and other molecules that are important in combustion and atmospheric chemistry, and extend high resolution spectroscopy to low frequency regions of the spectrum that can provide characteristic information on large molecules. The analyses of the spectra will also provide precise molecular parameters that can serve as experimental ?gold standards? to guide and benchmark electronic structure calculations. The broader scientific impacts of the proposed studies include valuable spectral data and diagnostics relevant to tropospheric chemistry, astrochemistry, and biochemistry. In addition, the young researchers working on these projects will acquire excellent training in physical chemistry - gaining invaluable experience in both sophisticated experimental and theoretical methods. Prof. Miller will continue the development of research-based graduate courses that emphasize the broad applications of molecular spectroscopy, as well as develop a new module on the same theme appropriate to introductory chemistry courses.