OD + CO -> DOCO动力学的直接频率梳测量
Direct Frequency Comb Measurement of OD + CO -> DOCO Kinetics
摘要：
OH + CO反应的动力学，大气和燃烧化学的基础，是复杂的，由于HOCO中间体的形成。尽管对该反应进行了广泛的研究，但在热反应条件下尚未观察到HOCO。利用时间分辨腔增强直接频率梳状光谱的灵敏，宽带和高分辨率的能力，我们观察OD + CO反应动力学与检测稳定的trans-DOCO，trans-HOCO的氘代类似物，及其产量。通过同时测量的时间依赖性浓度的trans-DOCO和OD物种，我们观察到明确的低压三分子依赖于反应速率系数为N2和CO浴气体。这些结果证实了HOCO的形成机理并量化了其产率。
英文摘要：
The kinetics of the OH + CO reaction, fundamental to both atmospheric and combustion chemistry, are complex due to the formation of the HOCO intermediate. Despite extensive studies on this reaction, HOCO has not been observed at thermal reaction conditions. Exploiting the sensitive, broadband, and high-resolution capabilities of time-resolved cavity-enhanced direct frequency comb spectroscopy, we observe OD + CO reaction kinetics with the detection of stabilized trans-DOCO, the deuterated analogue of trans-HOCO, and its yield. By simultaneously measuring the time-dependent concentrations of both trans-DOCO and OD species, we observe unambiguous low-pressure termolecular dependence on the reaction rate coefficients for both N2 and CO bath gases. These results confirm the HOCO formation mechanism and quantify its yield.
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