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Simultaneous determination of transient free radicals and reaction kinetics by high-resolution time-resolved dual-comb spectroscopy
Communications Chemistry ( IF 5.9 ) Pub Date : 2020-07-30 , DOI: 10.1038/s42004-020-00353-6
Pei-Ling Luo, Er-Chien Horng

Quantitative determination of multiple transient species is critical in investigating reaction mechanisms and kinetics under various conditions. Dual-comb spectroscopy, a comb-laser-based multi-heterodyne interferometric technique that enables simultaneous achievement of broadband, high-resolution, and rapid spectral acquisition, opens a new era of time-resolved spectroscopic measurements. Employing an electro-optic dual-comb spectrometer with central wavelength near 3 µm coupled with a Herriott multipass absorption cell, here we demonstrate simultaneous determination of multiple species, including methanol, formaldehyde, HO2 and OH radicals, and investigate the reaction kinetics. In addition to quantitative spectral analyses of high-resolution and tens of microsecond time-resolved spectra recorded upon flash photolysis of precursor mixtures, we determine a rate coefficient of the HO2 + NO reaction by directly detecting both HO2 and OH radicals. Our approach exhibits potential in discovering reactive intermediates and exploring complex reaction mechanisms, especially those of radical-radical reactions.



中文翻译:

通过高分辨率时间分辨双梳光谱同时测定瞬态自由基和反应动力学

多种瞬态物质的定量测定对于研究各种条件下的反应机制和动力学至关重要。双梳状光谱是一种基于梳状激光的多外差干涉技术,能够同时实现宽带、高分辨率和快速光谱采集,开启了时间分辨光谱测量的新时代。我们采用中心波长接近 3 µm 的电光双梳状光谱仪与 Herriott 多通道吸收池相结合,在这里我们展示了同时测定多种物质,包括甲醇、甲醛、HO 2和 OH 自由基,并研究反应动力学。除了对前体混合物的闪光光解记录的高分辨率和数十微秒时间分辨光谱进行定量光谱分析外,我们还 通过直接检测 HO 2和 OH 自由基来确定 HO 2 + NO 反应的速率系数。我们的方法在发现活性中间体和探索复杂反应机制方面具有潜力,尤其是自由基反应的机制。

更新日期:2020-07-30
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