Vibrational Relaxation of Highly Vibrationally Excited CO Scattered from Au(111): Evidence for CO– Formation,The Journal of Physical Chemistry Letters

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Vibrational Relaxation of Highly Vibrationally Excited CO Scattered from Au(111): Evidence for CO– Formation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-09-26 00:00:00 , DOI: 10.1021/acs.jpclett.7b02207
Roman J. V. Wagner ₁ , Niklas Henning ₁ , Bastian C. Krüger ₁ , G. Barratt Park _{1,

2} , Jan Altschäffel _{1,

2} , Alexander Kandratsenka ₂ , Alec M. Wodtke _{1,

2,

3} , Tim Schäfer ₁

Affiliation

Electronically nonadiabatic dynamics can be important in collisions of molecules at surfaces; for example, when vibrational degrees of freedom of molecules are coupled to electron-hole-pair (EHP) excitation of a metal. Such dynamics have been inferred from a host of observations involving multiquantum relaxation of NO molecules scattered from metal surfaces. Electron transfer forming transient NO^– is thought to be essential to the nonadiabatic coupling. The question remains: is this behavior usual? Here, we present final vibrational state distributions resulting from the scattering of CO(v_i = 17) from Au(111), which exhibits significantly less vibrational relaxation than NO(v_i = 16). We explain this observation in terms of the lower electron affinity of CO compared to NO, a result that is consistent with the formation of a transient CO^– ion being important to CO vibrational relaxation.

中文翻译：

高振动激发态CO的振动弛豫由Au散（111）：证据CO ^-形成

电子非绝热动力学在表面分子碰撞中很重要。例如，当分子的振动自由度与金属的电子空穴对（EHP）激发耦合时。这种动力学是从许多观察结果中推断出来的，这些观察结果涉及从金属表面散射的NO分子的多量子弛豫。电子传递形成瞬态NO ^–被认为是非绝热耦合必不可少的。问题仍然存在：这种行为是否正常？这里，从CO的散射导致我们当前最终振动状态分布（v_我= 17）由Au（111），其表现出小于显著振动弛豫比NO（v_我= 16）。我们解释这种观察相比NO，结果是与瞬态CO的形成一致的CO的低的电子亲合性方面^-离子为至CO振动弛豫重要。

更新日期：2017-09-26

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