Influence of caged noble-gas atom on the superatomic and valence states of C60−
Influence of caged noble-gas atom on the superatomic and valence states of C60−
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DOI：
10.1080/00268976.2015.1060367
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发表时间：
2015-07
影响因子：
1.7
通讯作者：
E. V. Gromov;S. Klaiman;L. Cederbaum
中科院分区：
文献类型：
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作者：
E. V. Gromov;S. Klaiman;L. Cederbaum
利用高能级从头算耦合团簇方法，对两种内富勒烯阴离子He@C−60和Ne@C−60进行了详细的研究。重点阐述了惰性气体原子对母体C-−-60稳定阴离子态的能量和电子结构的影响。我们的研究表明，惰性气体原子对C-−-60的类价态没有影响，但对类超原子的2Ag态有强烈的影响。后者在He@C−60和Ne@C−60物种中都经历了明显的不稳定，失去了超过70%的原始电子结合能。观察到的失稳是由于笼中的稀有气体原子扰动了笼内2Ag态的过剩电子密度。我们展示了我们的分析结果如何用于预测其他闭合壳层内面体络合物中2AG态的行为。讨论了观察到的2AG态特征的一些可能的含义。
Using high-level ab initio coupled cluster methods, we have conducted a detailed study of two endofullerene anions, He@C−60 and Ne@C−60. The main focus was on elucidating the effect of the noble-gas atom on the energy and electronic structure of the stable anion states of the parent C−60. Our study revealed that the noble-gas atom has no influence on the valence-like states of C−60, but strongly affects the superatomic-like 2Ag state. The latter was found to undergo pronounced destabilisation in both the He@C−60 and Ne@C−60 species, losing more than 70% of its original electron binding energy. The observed destabilisation is due to perturbation of the excess electron density of the 2Ag state inside the C60 cage by the caged noble-gas atom. We show how the results of our analysis can be used to predict the behaviour of the 2Ag state in other closed-shell endohedral complexes. Some possible implications of the observed features of the 2Ag state are discussed.