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Ultrafast dynamics of low-energy electron attachment via a non-valence correlation-bound state
Nature Chemistry ( IF 21.8 ) Pub Date : 2018-01-08 , DOI: 10.1038/nchem.2912
Joshua P. Rogers , Cate S. Anstöter , Jan R. R. Verlet

The primary electron-attachment process in electron-driven chemistry represents one of the most fundamental chemical transformations with wide-ranging importance in science and technology. However, the mechanistic detail of the seemingly simple reaction of an electron and a neutral molecule to form an anion remains poorly understood, particularly at very low electron energies. Here, time-resolved photoelectron imaging was used to probe the electron-attachment process to a non-polar molecule using time-resolved methods. An initially populated diffuse non-valence state of the anion that is bound by correlation forces evolves coherently in 30 fs into a valence state of the anion. The extreme efficiency with which the correlation-bound state serves as a doorway state for low-energy electron attachment explains a number of electron-driven processes, such as anion formation in the interstellar medium and electron attachment to fullerenes.



中文翻译:

低价电子通过非价相关束缚态的超快动力学

电子驱动化学中的主要电子附着过程代表了最基本的化学转化之一,在科学和技术中具有广泛的重要性。然而,关于电子和中性分子形成阴离子的看似简单反应的机理细节仍然知之甚少,特别是在电子能量非常低的情况下。在这里,时间分辨光电子成像被用来利用时间分辨方法探测电子与非极性分子的结合过程。由相关力约束的阴离子的初始填充的扩散非价态在〜内连贯地发展30 fs变成阴离子的价态。相关束缚态用作低能电子附着的门口状态的极高效率解释了许多电子驱动的过程,例如星际介质中的阴离子形成和电子与富勒烯的附着。

更新日期:2018-01-08
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