Nuñez-Reyes Dianailys, Bray Cédric, Hickson Kevin M, Larrégaray Pascal, Bonnet Laurent, González-Lezana Tomás
Université de Bordeaux, Institut des Sciences Moléculaires, F-33400 Talence, France.
Instituto de Física Fundamental, CSIC, IFF-CSIC Serrano 123, 28006 Madrid, Spain.
Phys Chem Chem Phys. 2020 Oct 28;22(41):23609-23617. doi: 10.1039/d0cp03971c.
This study reports the results of an experimental and theoretical investigation of the N(2D) + H2 and N(2D) + D2 reactions at room temperature and below. On the experimental side, a supersonic flow (Laval nozzle) reactor was employed to measure rate constants for these processes at temperatures as low as 127 K. N(2D) was produced indirectly by pulsed laser photolysis and these atoms were detected directly by pulsed laser induced fluorescence in the vacuum ultraviolet wavelength region. On the theoretical side, two different approaches were used to calculate rate constants for these reactions; a statistical quantum mechanical (SQM) method and a quasi-classical trajectory capture model including a semi-classical correction for tunneling (SC-Capture). This work is described in the context of previous studies, while the discrepancies between both experiment and theory, as well as between the theoretical results themselves are discussed.
本研究报告了在室温及以下温度下对N(2D) + H2和N(2D) + D2反应进行实验和理论研究的结果。在实验方面，采用了超声速流动（拉瓦尔喷嘴）反应器来测量这些过程在低至127 K温度下的速率常数。N(2D)通过脉冲激光光解间接产生，这些原子通过真空紫外波长区域的脉冲激光诱导荧光直接检测。在理论方面，使用了两种不同的方法来计算这些反应的速率常数；一种统计量子力学（SQM）方法和一种包括隧穿半经典校正的准经典轨迹捕获模型（SC-Capture）。这项工作是在先前研究的背景下进行描述的，同时讨论了实验与理论之间以及理论结果本身之间的差异。
