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Hydroxyl Radical Fluorescence and Quantum Yield Following Lyman-α Photoexcitation of Water Vapor in a Room Temperature Cell and Cooled in a Supersonic Expansion
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-06-05 00:00:00 , DOI: 10.1021/acs.jpca.8b03047 Justin W. Young 1, 2 , Ryan S. Booth 1, 2 , Kristen M. Vogelhuber 1, 2 , Jaime A. Stearns 1 , Christopher J. Annesley 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-06-05 00:00:00 , DOI: 10.1021/acs.jpca.8b03047 Justin W. Young 1, 2 , Ryan S. Booth 1, 2 , Kristen M. Vogelhuber 1, 2 , Jaime A. Stearns 1 , Christopher J. Annesley 1
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Photoexcitation of water by Lyman-α (121.6 nm) induces a dissociation reaction that produces OH(A2Σ+) + H. Despite this reaction being part of numerous studies, a combined understanding of the product and fluorescence yields is still lacking. Here, the rotational and vibrational distributions of OH(A) are determined from dispersed fluorescence following photoexcitation of both room-temperature and jet-cooled water vapor, for the first time in the same experiment. This work compares new data of state-resolved fluorescence with literature molecular branching ratios and brings previous studies into agreement through careful consideration of OH(A) fluorescent and predissociation lifetimes and confirms a fluorescent quantum yield of 8%. Comparison of the room-temperature and jet-cooled OH(A) populations indicate the temperature of H2O prior to excitation has subtle effects on the OH(A) population distribution, such as altering the rotational distribution in the ν′ = 0 population and affecting the population in the ν′ = 1 state. These results indicate jet-cooled water vapor may have a 1% higher fluorescence quantum yield compared to room-temperature water vapor.
中文翻译：
Lyman-α光激发室温室内水蒸气并以超音速膨胀冷却后的羟基自由基荧光和量子产率
通过莱曼-α（121.6纳米）的光激发水诱导产生OH（A的解离反应2 Σ +）+H。尽管该反应是众多研究的一部分，但仍缺乏对产物和荧光产率的综合理解。在此，在同一实验中首次从室温和射流冷却的水蒸气的光激发后，从分散的荧光确定OH（A）的旋转和振动分布。这项工作将状态分辨荧光的新数据与文献中的分子支化比率进行了比较，并通过仔细考虑OH（A）荧光和预离解寿命，使先前的研究取得了一致，并确认了8％的荧光量子产率。室温和喷射冷却的OH（A）族群的比较表明H 2的温度激发之前的O对OH（A）种群分布具有微妙的影响，例如改变ν'= 0种群中的旋转分布并影响ν'= 1状态下的种群。这些结果表明，与室温水蒸气相比，射流冷却的水蒸气的荧光量子产率可能高1％。
更新日期：2018-06-05
中文翻译：
Lyman-α光激发室温室内水蒸气并以超音速膨胀冷却后的羟基自由基荧光和量子产率
通过莱曼-α（121.6纳米）的光激发水诱导产生OH（A的解离反应2 Σ +）+H。尽管该反应是众多研究的一部分，但仍缺乏对产物和荧光产率的综合理解。在此，在同一实验中首次从室温和射流冷却的水蒸气的光激发后，从分散的荧光确定OH（A）的旋转和振动分布。这项工作将状态分辨荧光的新数据与文献中的分子支化比率进行了比较，并通过仔细考虑OH（A）荧光和预离解寿命，使先前的研究取得了一致，并确认了8％的荧光量子产率。室温和喷射冷却的OH（A）族群的比较表明H 2的温度激发之前的O对OH（A）种群分布具有微妙的影响，例如改变ν'= 0种群中的旋转分布并影响ν'= 1状态下的种群。这些结果表明，与室温水蒸气相比，射流冷却的水蒸气的荧光量子产率可能高1％。
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