Actinide-embedded gold superatom models: Electronic structure, spectroscopic properties, and applications in surface-enhanced Raman scattering
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- 作者：Yang Gao ; Bo Wang ; Yanyu Lei ; Boon K. Teo ; Zhigang Wang
- 关键词：actinide element ; DFT calculation ; gold nanoparticle ; superatomic orbital ; surface ; enhanced Raman scattering
- 刊名：Nano Research
- 出版年：2016
- 出版时间：March 2016
- 年：2016
- 卷：9
- 期：3
- 页码：622-632
- 全文大小：1,962 KB
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Bo Wang (1) (2)
Yanyu Lei (1) (2)
Boon K. Teo (3) (4)
Zhigang Wang (1) (2) (5)
1. Institute of Atomic and Molecular Physics, Jilin University, Changchun, 130012, China
2. Jilin Provincial Key Laboratory of Applied Atomic and Molecular Spectroscopy, Jilin University, Changchun, 130012, China
3. College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China
4. College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
5. Beijing Computational Science Research Center, Beijing, 100084, China - 刊物类别：Chemistry and Materials Science
- 刊物主题：Chinese Library of Science
Chemistry
Nanotechnology - 出版者：Tsinghua University Press, co-published with Springer-Verlag GmbH
- ISSN：1998-0000
文摘
Actinide elements encaged in a superatomic cluster can exhibit unique properties due to their hyperactive valence electrons. Herein, the electronic and spectroscopic properties of Th@Au14 are predicted and compared with that of the isoelectronic entities [Ac@Au14]− and [Pa@Au14]+ using density functional theory. The calculation results indicate that these clusters all adopt a closedshell superatomic 18-electron configuration of the 1S21P61D10 Jellium state. The absorption spectrum of Th@Au14 can be interpreted by the Jelliumatic orbital model. In addition, calculated spectra of pyridine-Th@Au14 complexes in the blue laser band exhibit strong peaks attributable to charge transfer (CT) from the metal to the pyridine molecule. These charge-transfer bands lead to a resonant surface-enhanced Raman scattering (SERS) enhancement of ∼104. This work suggests a basis for designing and synthesizing SERS substrate materials based on actinide-embedded gold superatom models.