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NO + He 碰撞中能量相关的宇称-宇称对行为。

Energy dependent parity-pair behavior in NO + He collisions.

机构信息

Institute for Molecules and Materials, Radboud University, Heijendaalseweg 135, 6525 AJ Nijmegen, The Netherlands.

出版信息

J Chem Phys. 2018 Aug 28;149(8):084306. doi: 10.1063/1.5042074.

Abstract

Colliding molecules behave fundamentally differently at high and low collision energies. At high energies, a collision can be described to a large extent using classical mechanics, and the scattering process can be compared to a billiard-ball-like collision. At low collision energies, the wave character of the collision partners dominates, and only quantum mechanics can predict the outcome of an encounter. It is, however, not so clear how these limits evolve into each other as a function of the collision energy. Here, we investigate and visualize this evolution using a special feature of the differential cross sections for inelastic collisions between NO radicals and He atoms. The so-called "parity-pair" transitions have similar differential cross sections at high collision energies, whereas their cross sections are significantly different in the quantum regime at low energies. These transitions can be used as a probe for the quantum nature of the collision process. The similarity of the parity-pair differential cross sections at high energies could be theoretically explained if the first-order Born approximation were applicable. We found, however, that the anisotropy of the NO-He interaction potential is too strong for the first-order Born approximation to be valid, so higher-order perturbations must be taken into account.

摘要

在高能量和低能量碰撞时,碰撞分子的行为存在根本差异。在高能量下,碰撞在很大程度上可以用经典力学来描述,散射过程可以类比为台球碰撞。在低能量碰撞时,碰撞伙伴的波动性占主导地位,只有量子力学才能预测碰撞的结果。然而,随着碰撞能量的变化,这些极限如何相互演变并不清楚。在这里,我们使用 NO 自由基和 He 原子之间非弹性碰撞的微分截面的一个特殊特征来研究和可视化这种演变。所谓的“宇称对”跃迁在高能量碰撞时具有相似的微分截面,而在低能量量子区域,它们的截面则有显著差异。这些跃迁可以作为碰撞过程量子性质的探针。如果适用一级玻恩近似,那么在高能量时宇称对微分截面的相似性可以从理论上解释。然而,我们发现,NO-He 相互作用势能的各向异性太强,以至于一级玻恩近似不成立,因此必须考虑更高阶的微扰。

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