High Resolution Spectroscopy of Reactive Chemical Intermediates and Related Studies

本课题由化学系化学结构、动力学和机理研究计划资助，Terry A。俄亥俄州州立大学的米勒和他的研究小组将利用高分辨率光腔衰荡光谱（HR-CRDS）获得和分析与对流层化学有关的许多反应性化学中间体的光谱，包括有机过氧自由基、硝酸根和羟基烷氧基自由基。米勒实验室开发的一种称为远红外/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（与天体化学有关）和氨基酸等生物相关分子的高分辨率光谱。这些研究将为燃烧和大气化学中重要的自由基和其他分子提供诊断标记，并将高分辨率光谱学扩展到可以提供大分子特征信息的光谱低频区域。光谱的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有关的宝贵光谱数据和诊断。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。米勒教授将继续发展以研究为基础的研究生课程，强调分子光谱学的广泛应用，以及开发一个新的模块在同一主题适合介绍化学课程。

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.