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氩二聚体中氩原子共振核心激发后的原子间库仑衰变

Interatomic Coulombic decay following resonant core excitation of Ar in argon dimer.

作者信息

Miteva T, Chiang Y-C, Kolorenč P, Kuleff A I, Gokhberg K, Cederbaum L S

机构信息

Theoretische Chemie, Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany.

Institute of Theoretical Physics, Faculty of Mathematics and Physics, Charles University in Prague, V Holešovičkách 2, 180 00 Prague, Czech Republic.

出版信息

J Chem Phys. 2014 Aug 14;141(6):064307. doi: 10.1063/1.4891986.

Abstract

A scheme utilizing excitation of core electrons followed by the resonant-Auger - interatomic Coulombic decay (RA-ICD) cascade was recently proposed as a means of controlling the generation site and energies of slow ICD electrons. This control mechanism was verified in a series of experiments in rare gas dimers. In this article, we present fully ab initio computed ICD electron and kinetic energy release spectra produced following 2p(3/2) → 4s, 2p(1/2) → 4s, and 2p(3/2) → 3d core excitations of Ar in Ar2. We demonstrate that the manifold of ICD states populated in the resonant Auger process comprises two groups. One consists of lower energy ionization satellites characterized by fast interatomic decay, while the other consists of slow decaying higher energy ionization satellites. We show that accurate description of nuclear dynamics in the latter ICD states is crucial for obtaining theoretical electron and kinetic energy release spectra in good agreement with the experiment.

摘要

最近提出了一种利用核心电子激发随后进行共振俄歇 - 原子间库仑衰变(RA - ICD)级联的方案,作为控制慢ICD电子产生位置和能量的一种手段。这种控制机制在一系列稀有气体二聚体实验中得到了验证。在本文中,我们展示了在Ar₂中对Ar进行2p(3/2)→4s、2p(1/2)→4s和2p(3/2)→3d核心激发后从头计算得到的ICD电子和动能释放光谱。我们证明,在共振俄歇过程中填充的ICD态流形包括两组。一组由以快速原子间衰变为特征的低能量电离卫星组成,而另一组由缓慢衰变的高能量电离卫星组成。我们表明,对后一种ICD态中的核动力学进行准确描述对于获得与实验良好吻合的理论电子和动能释放光谱至关重要。

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