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金属表面基态正氢解离的旋转取向控制

Rotational orientation control of a ground state ortho-H dissociation on a metal surface.

作者信息

Chadwick H, Zhang G, Baker C J, Smith P L, Alexandrowicz G

机构信息

Department of Chemistry, Faculty of Science and Engineering, Swansea University, Swansea, UK.

出版信息

Nat Commun. 2025 May 19;16(1):4625. doi: 10.1038/s41467-025-59928-3.

Abstract

When hydrogen molecules collide with a surface, they can either scatter away from the surface or undergo dissociative chemisorption. The relative probabilities of these different outcomes could depend on the rotational orientation of the impinging molecules, however, due to the lack of steric control techniques for ground state hydrogen, they could not be measured directly. Here, we demonstrate that magnetic field manipulation can be used to control the rotational orientation of H molecules colliding with a nickel surface and change the balance between reactive and scattering collision events. Our measurements show that molecules which approach the surface while rotating within a plane parallel to the surface are less likely to undergo specular scattering than those rotating within a perpendicular plane. An opposite trend was measured for the likelihood of dissociative chemisorption. A possible link between these two findings, and its potential impact on the interpretation of dissociation mechanisms is discussed.

摘要

当氢分子与表面碰撞时,它们要么从表面散射开,要么发生解离化学吸附。然而,这些不同结果的相对概率可能取决于入射分子的旋转取向,由于缺乏针对基态氢的空间控制技术,无法直接测量这些概率。在此,我们证明磁场操纵可用于控制与镍表面碰撞的氢分子的旋转取向,并改变反应性碰撞事件和散射碰撞事件之间的平衡。我们的测量结果表明,在与表面平行的平面内旋转时接近表面的分子比在垂直平面内旋转的分子发生镜面反射散射的可能性更小。对于解离化学吸附的可能性,测量到了相反的趋势。讨论了这两个发现之间可能的联系及其对解离机制解释的潜在影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6bee/12089284/604e156f5be6/41467_2025_59928_Fig1_HTML.jpg

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