Actinide-embedded gold superatom models: Electronic structure, spectroscopic properties, and applications in surface-enhanced Raman scattering

作者：Gao, Yang; Wang, Bo; Lei, Yanyu; Teo, Boon K.^*; Wang, Zhigang^*

来源：Nano Research, 2016, 9(3): 622-632.

DOI：10.1007/s12274-015-0942-4

• actinide element
• DFT calculation
• gold nanoparticle
• superatomic orbital
• surface-enhanced Raman scattering

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@Au-14 are predicted and compared with that of the isoelectronic entities [Ac@Au-14](-) and [Pa@Au-14](+) using density functional theory. The calculation results indicate that these clusters all adopt a closedshell superatomic 18-electron configuration of the 1S(2)1P(6)1D(10) Jellium state. The absorption spectrum of Th@Au-14 can be interpreted by the Jelliumatic orbital model. In addition, calculated spectra of pyridine-Th@Au-14 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 similar to 10(4). This work suggests a basis for designing and synthesizing SERS substrate materials based on actinide-embedded gold superatom models.

• 出版日期2016-3
• 单位厦门大学; 北京大学; 北京计算科学研究中心; 吉林大学