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在 H+HD→H+D 反应中直接观察前向散射振荡。

Direct observation of forward-scattering oscillations in the H+HD→H+D reaction.

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, China.

Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou, China.

出版信息

Nat Chem. 2018 Jun;10(6):653-658. doi: 10.1038/s41557-018-0032-9. Epub 2018 Apr 23.

Abstract

Accurate measurements of product state-resolved angular distributions are central to fundamental studies of chemical reaction dynamics. Yet, fine quantum-mechanical structures in product angular distributions of a reactive scattering process, such as the fast oscillations in the forward-scattering direction, have never been observed experimentally and the nature of these oscillations has not been fully explored. Here we report the crossed-molecular-beam experimental observation of these fast forward-scattering oscillations in the product angular distribution of the benchmark chemical reaction, H + HD → H + D. Clear oscillatory structures are observed for the H(v' = 0, j' = 1, 3) product states at a collision energy of 1.35 eV, in excellent agreement with the quantum-mechanical dynamics calculations. Our analysis reveals that the oscillatory forward-scattering components are mainly contributed by the total angular momentum J around 28. The partial waves and impact parameters responsible for the forward scatterings are also determined from these observed oscillations, providing crucial dynamics information on the transient reaction process.

摘要

准确测量产物态分辨角分布对于化学反应动力学的基础研究至关重要。然而,反应散射过程中产物角分布的精细量子力学结构,例如前向散射方向的快速振荡,从未在实验中观察到过,这些振荡的性质也尚未得到充分探索。在这里,我们报告了在基准化学反应 H + HD → H + D 的产物角分布中交叉分子束实验观测到的这些快速前向散射振荡。在 1.35eV 的碰撞能下,清晰地观察到了 H(v'=0, j'=1, 3)产物态的振荡结构,与量子力学动力学计算结果非常吻合。我们的分析表明,振荡的前向散射分量主要由总角动量 J 贡献,约为 28。这些观察到的振荡还确定了前向散射的部分波和碰撞参数,为瞬态反应过程提供了关键动力学信息。

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