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自旋轨道分裂分波之间在 F + HD → HF + D 反应中的量子干涉。

Quantum interference between spin-orbit split partial waves in the F + HD → HF + D reaction.

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China.

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

出版信息

Science. 2021 Feb 26;371(6532):936-940. doi: 10.1126/science.abf4205.

Abstract

The effect of electron spin-orbit interactions on chemical reaction dynamics has been a topic of much research interest. Here we report a combined experimental and theoretical study on the effect of electron spin and orbital angular momentum in the F + HD → HF + D reaction. Using a high-resolution imaging technique, we observed a peculiar horseshoe-shaped pattern in the product rotational-state-resolved differential cross sections around the forward-scattering direction. The unusual dynamics pattern could only be explained properly by highly accurate quantum dynamics theory when full spin-orbit characteristics were considered. Theoretical analysis revealed that the horseshoe pattern was largely the result of quantum interference between spin-orbit split-partial-wave resonances with positive and negative parities, providing a distinctive example of how spin-orbit interaction can effectively influence reaction dynamics.

摘要

电子自旋-轨道相互作用对化学反应动力学的影响一直是许多研究关注的主题。在这里,我们报告了一个关于 F + HD → HF + D 反应中电子自旋和轨道角动量影响的实验和理论综合研究。我们使用高分辨率成像技术,在正向散射方向附近的产物转动态分辨微分截面中观察到了一种特殊的马蹄形图案。只有当考虑到完整的自旋-轨道特性时,高度精确的量子动力学理论才能正确解释这种异常动力学模式。理论分析表明,马蹄形图案主要是自旋轨道分裂分波共振的正负宇称之间的量子干涉的结果,为自旋轨道相互作用如何有效地影响反应动力学提供了一个独特的例子。

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