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一种均匀流腔衰荡光谱仪(UF-CRDS):一种用于低温光谱学和动力学研究的新装置。

A uniform flow-cavity ring-down spectrometer (UF-CRDS): A new setup for spectroscopy and kinetics at low temperature.

机构信息

Department of Chemistry, University of Missouri, Columbia, Missouri 65211, USA.

出版信息

J Chem Phys. 2019 Dec 28;151(24):244202. doi: 10.1063/1.5125574.

Abstract

The UF-CRDS (Uniform Flow-Cavity Ring Down Spectrometer) is a new setup coupling for the first time a pulsed uniform (Laval) flow with a continuous wave CRDS in the near infrared for spectroscopy and kinetics at low temperature. This high resolution and sensitive absorption spectrometer opens a new window into the phenomena occurring within UFs. The approach extends the detection range to new electronic and rovibrational transitions within Laval flows and offers the possibility to probe numerous species which have not been investigated yet. This new tool has been designed to probe radicals and reaction intermediates but also to follow the chemistry of hydrocarbon chains and PAHs which play a crucial role in the evolution of astrophysical environments. For kinetics measurements, the UF-CRDS combines the CRESU technique (French acronym meaning reaction kinetics in uniform supersonic flows) with the SKaR (Simultaneous Kinetics and Ring-Down) approach where, as indicated by its name, the entire reaction is monitored during each intensity decay within the high finesse cavity. The setup and the approach are demonstrated with the study of the reaction between CN (v = 1) and propene at low temperature. The recorded data are finally consistent with a previous study of the same reaction for CN (v = 0) relying on the CRESU technique with laser induced fluorescence detection.

摘要

UF-CRDS(均匀流-腔衰荡光谱仪)是一种新的装置,首次将脉冲均匀(拉瓦尔)流与连续波 CRDS 耦合在一起,用于低温下的光谱学和动力学研究。这种高分辨率和高灵敏度的吸收光谱仪为研究 UFs 内部发生的现象开辟了新的窗口。该方法将检测范围扩展到了拉瓦尔流中全新的电子和转动跃迁,并提供了探测尚未研究过的众多物质的可能性。该新工具旨在探测自由基和反应中间体,但也可以跟踪在天体物理环境演化中起着关键作用的碳氢链和多环芳烃的化学变化。对于动力学测量,UF-CRDS 将 CRESU 技术(法语缩写,意为均匀超音速流中的反应动力学)与 SKaR(同时动力学和衰荡)方法相结合,正如其名称所示,在高精细度腔的每次强度衰减期间,整个反应都被监测。通过低温下 CN(v=1)与丙烯反应的研究,展示了该装置和方法。记录的数据最终与之前基于 CRESU 技术和激光诱导荧光检测的同一反应的 CN(v=0)的研究结果一致。

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