Interatomic Coulombic Decay Mediated by Ultrafast Superexchange Energy Transfer
Interatomic Coulombic Decay Mediated by Ultrafast Superexchange Energy Transfer
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DOI：
10.1103/physrevlett.119.083403
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发表时间：
2017-08-25
影响因子：
8.6
通讯作者：
Sisourat, Nicolas
中科院分区：
文献类型：
--
作者：
Miteva, Tsveta;Kazandjian, Sevan;Sisourat, Nicolas
由于原子间库仑衰变（ICD）的超快去激发的可能性，原子和分子的内价电离态在嵌入环境中的寿命较短。在这篇论文中，我们表明，当桥原子靠近两个相互作用的单体时，这些ICD活性态的寿命进一步降低。这种新机制被称为超交换ICD，是一种由桥原子虚态的有效能量转移驱动的电子相关效应。以NeHeNe三聚体为例，详细讨论了超交换ICD。我们证明了在He原子存在时，Ne+ (2s(-1)) (2)Sigma(+)(g)共振的衰减宽度增加了6倍，并且在两个Ne原子之间的距离为4埃。利用一个简单的模型，我们给出了超交换ICD的定性解释，并推导出了衰变宽度与氖原子间距离关系的解析表达式。
Inner-valence ionized states of atoms and molecules live shorter if these species are embedded in an environment due to the possibility for ultrafast deexcitation known as interatomic Coulombic decay (ICD). In this Letter we show that the lifetime of these ICD active states decreases further when a bridge atom is in proximity to the two interacting monomers. This novel mechanism, termed superexchange ICD, is an electronic correlation effect driven by the efficient energy transfer via virtual states of the bridge atom. The superexchange ICD is discussed in detail on the example of the NeHeNe trimer. We demonstrate that the decay width of the Ne+ (2s(-1)) (2)Sigma(+)(g) resonance increases 6 times in the presence of the He atom at a distance of 4 angstrom between the two Ne atoms. Using a simple model, we provide a qualitative explanation of the superexchange ICD and we derive analytical expressions for the dependence of the decay width on the distance between the neon atoms.