Bhattacharyya Surjendu, Mondal Sohidul, Liu Kopin
Institute of Atomic and Molecular Sciences (IAMS) , Academia Sinica , P.O. Box 23-166, Taipei , 10617 , Taiwan.
Department of Physics , National Taiwan University , Taipei , 10617 , Taiwan.
J Phys Chem Lett. 2018 Sep 20;9(18):5502-5507. doi: 10.1021/acs.jpclett.8b02517. Epub 2018 Sep 11.
The title reaction was studied in a crossed-beam scattering experiment at the collisional energy ( E) ranging from 0.46 to 4.53 kcal mol. Using a time-sliced velocity-imaging technique, both the pair-correlated integral and differential cross sections were measured. On the basis of the observed structures in state-specific excitation functions and the patterns in the E evolution of product angular distributions, we inferred that the title reaction proceeds predominantly via a resonance-mediated pathway, in contrast to the previous findings in the isotopically analogous reactions where the alternative direct abstraction pathway often dominates the reactivity. Despite the complexity of numerous scattering resonances involved in this six-atom reaction, extending our understanding of the isolated resonance in the analogous benchmark F + HD (H) reaction enables us to propose plausible mechanistic origins for the formation as well as the decay of the complicated overlapped resonances.
在碰撞能量(E)范围为0.46至4.53千卡/摩尔的交叉束散射实验中研究了该标题反应。使用时间切片速度成像技术,测量了对关联积分截面和微分截面。基于在特定状态激发函数中观察到的结构以及产物角分布的E演化模式,我们推断该标题反应主要通过共振介导的途径进行,这与同位素类似反应中的先前发现相反,在同位素类似反应中,替代的直接提取途径通常主导反应性。尽管这个六原子反应涉及众多散射共振的复杂性,但扩展我们对类似基准F + HD(H)反应中孤立共振的理解,使我们能够为复杂重叠共振的形成和衰减提出合理的机理起源。