期刊
ACS NANO
卷 14, 期 6, 页码 6599-6606出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c01000
关键词
alloy nanoclusters; atomic precision; dipole moment; dipole-dipole interaction; controlled assembly
类别
资金
- National Science Foundation [NSF DMR-1808675]
- Air Force Office of Scientific Research (AFOSR) [FA9550-171-0099]
- NSF [ACI-1548562]
- National Science Foundation (CBET-CAREER program) [1652694]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1652694] Funding Source: National Science Foundation
Dipole moment (mu) is a critical parameter for molecules and nanomaterials as it affects many properties. In metal-thiolate (SR) nanoclusters (NCs), pi is commonly low (0-5 D) compared to quantum dots. Herein, we report a doping strategy to give giant dipoles (similar to 18 D) in M-23 (M = Au/Ag/Cd) NCs, falling in the experimental trend for II-VI quantum dots. In M-23 NCs, high it is caused by the Cd-Br bond and the arrangement of heteroatoms along the C-3 axis. Strong dipole-dipole interactions are observed in crystalline state, with energy exceeding 5 kJ/mol, directing a head-to-tail alignment of Au22-nAgnCd1(SR)(15)X (SR = adamantanethiolate) dipoles. The alignment can be controlled by mu via doping. The optical absorption peaks of M-23 show solvent polarity-dependent shifts (similar to 25 meV) with negative solvatochromism. Detailed electronic structures of M-23 are revealed by density functional theory and time-dependent DFT calculations. Overall, the doping strategy for obtaining large dipole moments demonstrates an atomic-level design of clusters with useful properties.
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