Li Jiarui, Wang Rui, Huang Wanrong, Zhu Yu, Teo Boon K, Wang Zhigang
Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China.
College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
J Phys Chem Lett. 2023 Mar 23;14(11):2862-2868. doi: 10.1021/acs.jpclett.3c00445. Epub 2023 Mar 15.
This work reports a series of endohedral metallofullerene superatoms [Mg@C], where = 4, 2, 0, -2, and -4. It was found that Mg transfers virtually all of its 3s electrons to the C shell, resulting in the ionic states of Mg@[C]. Detailed calculations revealed that the superatomic electronic configuration of these clusters is 1S1P1D1F. The first nine superatomic molecular orbitals (SAMOs), 1S1P1D, housed with 18 electrons, are largely based on [C] with small contributions from magnesium, while the outmost SAMOs, 1F, with 4 - extra electrons, reside solely on [C]. The interaction between the Mg ion and [C] was found to be predominately ionic in character. Furthermore, ultraviolet-visible spectra provide a theoretical basis for fingerprinting these clusters. It is hoped that this work will encourage the synthetic pursuit of these smallest superatomic systems.
这项工作报道了一系列内嵌金属富勒烯超原子[Mg@C]，其中 = 4、2、0、-2和-4。研究发现，镁几乎将其所有3s电子转移到C壳层，从而形成Mg@[C]的离子态。详细计算表明，这些团簇的超原子电子构型为1S1P1D1F。前九个容纳18个电子的超原子分子轨道（SAMOs），即1S1P1D，主要基于[C]，镁的贡献较小，而最外层的SAMOs，即1F，带有4个额外电子，仅存在于[C]上。发现镁离子与[C]之间的相互作用主要是离子性的。此外，紫外可见光谱为识别这些团簇提供了理论基础。希望这项工作能激发对这些最小超原子体系的合成探索。
