富勒烯 Li@C 的电荷分离态。

Charge separated states of endohedral fullerene Li@C.

机构信息

Theoretical Chemistry, Institute of Physical Chemistry, University of Heidelberg, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany.

出版信息

J Chem Phys. 2019 Sep 21;151(11):114306. doi: 10.1063/1.5120017.

DOI:10.1063/1.5120017

PMID:31542008

Abstract

We report on high-level coupled-cluster calculations of electronic states of the neutral endohedral fullerene Li@C. All computed states of neutral Li@C are found to be the charge separated states of the Li@C type. Using the state-of-the-art EA-EOM-CCSD method, we found that neutral Li@C (D) possesses several valence and superatomic charge separated states with considerable electron binding energies, the strongest bound state of Li@C being the 1E state (6.73 eV). The valence charge separated states correspond to two sets of states of C . The states 1E, 1A, 2E, and 2A correspond to the respective bound states of C , and the states 2A, 1E, 1A, and 4E correspond to the unbound states of C . There are eight superatomic states with electron binding energy higher than 1.0 eV, being much stronger bound than the single weakly bound superatomic state of the parent fullerene anion. The analysis of the radial density distribution of the excess electron on the carbon cage indicates the important role of the inner part of the superatomic states in forming the charge separated states.

摘要

我们报告了中性笼状富勒烯 Li@C 的电子态的高水平耦合簇计算。发现中性 Li@C 的所有计算态都是 Li@C 型的电荷分离态。使用最先进的 EA-EOM-CCSD 方法，我们发现中性 Li@C(D) 具有几个具有相当大电子结合能的价和超原子电荷分离态，Li@C 的最强束缚态是 1E 态（6.73 eV）。价电荷分离态对应于 C 的两组态。态 1E、1A、2E 和 2A 对应于 C 的相应束缚态，而态 2A、1E、1A 和 4E 对应于 C 的非束缚态。有八个超原子态具有高于 1.0 eV 的电子结合能，比母体富勒烯阴离子的单个弱束缚超原子态强得多。对碳笼上过剩电子的径向密度分布的分析表明，超原子态的内部部分在形成电荷分离态中起着重要作用。