Structure Assignment, Electronic Properties, and Magnetism Quenching of Endohedrally Doped Neutral Silicon Clusters, SinCo (n = 10鈥?

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• 作者：Yejun Li ; Nguyen Minh Tam ; Pieterjan Claes ; Alex P. Woodham ; Jonathan T. Lyon ; Vu Thi Ngan ; Minh Tho Nguyen ; Peter Lievens ; Andr茅 Fielicke ; Ewald Janssens
• 刊名：Journal of Physical Chemistry A
• 出版年：2014
• 出版时间：September 18, 2014
• 年：2014
• 卷：118
• 期：37
• 页码：8198-8203
• 全文大小：286K
• ISSN：1520-5215

文摘

The structures of neutral cobalt-doped silicon clusters have been assigned by a combined experimental and theoretical study. Size-selective infrared spectra of neutral Si_nCo (n = 10鈥?2) clusters are measured using a tunable IR鈥揢V two-color ionization scheme. The experimental infrared spectra are compared with calculated spectra of low-energy structures predicted at the B3P86 level of theory. It is shown that the Si_nCo (n = 10鈥?2) clusters have endohedral caged structures, where the silicon frameworks prefer double-layered structures encapsulating the Co atom. Electronic structure analysis indicates that the clusters are stabilized by an ionic interaction between the Co dopant atom and the silicon cage due to the charge transfer from the silicon valence sp orbitals to the cobalt 3d orbitals. Strong hybridization between the Co dopant atom and the silicon host quenches the local magnetic moment on the encapsulated Co atom.