State-Resolved Spectroscopy and Dynamics of Chemical Transients

在这项由化学系实验物理化学计划资助的提案中，科罗拉多大学的大卫·内斯比特将继续开展一项使用状态分辨技术研究化学瞬变的光谱和动力学的计划。该项目将研究瞬变物质的光谱，量子态选择的反应动力学，以及询问喷射冷却瞬变物质的新方法的开发和开发。用直接吸收红外激光方法研究缝隙超音速放电中喷流冷却的自由基、分子离子和分子离子团簇。用IR-UV-UV三重共振法研究簇合物的高灵敏度泛音光谱以及与定向或定向试剂的反应动力学。利用新型光学外差/高精细腔方法与狭缝放电源相结合，将研究喷射冷却化学瞬变的超灵敏可见光吸收光谱。这项研究计划专注于在极高能量条件下产生的短寿命分子和离子，因此它们在自然界中通常不会以稳定的形式存在。这些研究除了具有基本的意义外，对于解决燃烧和大气化学以及天体物理化学方面的问题也具有实际意义。

In this proposal funded by the Experimental Physical Chemistry Program of the Chemistry Division, David Nesbitt of the University of Colorado will pursue a program of research on the spectroscopy and dynamics of chemical transients using state-resolved techniques. The project will examine the spectroscopy of transient species, quantum state-selected reaction dynamics, and the development and exploitation of new methods to interrogate jet-cooled transient species. Jet-cooled radicals, molecular ions, and molecular ion clusters will be investigated in slit supersonic discharges using direct absorption infrared laser methods. High sensitivity overtone spectroscopy of clusters and reaction dynamics with aligned or oriented reagents will be studied using IR-UV-UV triple resonance methods. The ultrasensitive visible absorption spectroscopy of jet-cooled chemical transients will be examined using novel optical heterodyne/high finesse cavity methods combined with slit discharge sources. This research program focuses on short-lived molecules and ions that are created under extremely energetic conditions, and thus they usually are not found in nature in stable forms. Besides being of fundamental interest, these studies have practical relevance to solving problems in combustion and atmospheric chemistry as well as in astrophysical chemistry.