Vibrationally inelastic scattering of HCl from Ag(111).
Vibrationally inelastic scattering of HCl from Ag(111).
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DOI：
10.1063/5.0026228
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发表时间：
2020-10
期刊：
影响因子：
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通讯作者：
Jan Geweke;A. Wodtke
中科院分区：
文献类型：
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作者：
Jan Geweke;A. Wodtke
利用分子束冷却样品和量子态选择探测技术，我们观察到HCl（v = 0）与Ag（111）表面碰撞时的v = 0 → 1振动跃迁，并导出了跃迁几率与入射能量和表面温度的关系.我们的观察表明，电子绝热和非绝热机制在这个非弹性过程中发挥作用。与其他系统的比较表明，与形成瞬态HCl-的电子转移机制一致的相似性和趋势。例如，电子非绝热耦合是强于HCl散射从Au，其中固体的功函数较高。HCl与其他体系的不同之处在于，在低势垒下可能发生解离。当HCl（v = 1）与Ag（111）面碰撞时，没有观察到振动非弹性的v = 1 → 2跃迁。我们建议，散射事件，其中HCl（v = 1）是受动力学的影响，增加其振动能量，导致有效地解离之前，HCl（v = 2）分子可以逃离表面。这个系统似乎是一个很好的候选人研究电子非绝热效应的解离吸附。
Using molecular beam cooled samples and quantum state-selective detection, we observe v = 0 → 1 vibrational transitions when HCl (v = 0) collides with an Ag(111) surface and derive both the incidence energy and surface temperature dependence of the transition probability. Our observations reveal that both electronically adiabatic and non-adiabatic mechanisms are at play in this inelastic process. A comparison to other systems shows similarities and trends that are consistent with an electron transfer mechanism forming a transient HCl-. For example, the electronically nonadiabatic coupling is stronger than for HCl scattering from Au, where the solid's work function is higher. HCl differs from other systems in that dissociation is possible over a low barrier. Vibrationally inelastic v = 1 → 2 transitions could not be seen when HCl (v = 1) collides with an Ag(111) surface. We suggest that scattering events, where HCl (v = 1) is subject to dynamical influences that increase its vibrational energy, lead efficiently to dissociation before the HCl (v = 2) molecule can escape the surface. This system appears to be an excellent candidate to study electronically nonadiabatic effects in dissociative adsorption.