期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 16, 页码 9038-9044出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202015907
关键词
nanoclusters; NIR-II photoluminescence; silver; single crystal X-ray structure; superatoms
资金
- Research Center Program of the IBS in Korea [IBS-R006-D1]
- Academy of Finland [292352, 294217, 319208]
- National Key R&D Program of China [2017YFA0207304]
- NSF of China [21890752, 21731005, 21721001]
The synthesis of atomically precise metalloid nanoclusters with distinct molecular structures remains challenging. This study successfully synthesized a charge-neutral silver nanocluster with specific ligands, resulting in enhanced photoluminescence quantum yield compared to other nanoclusters. The structural effects on the optical properties were significantly influenced by the unique electronic structure of the Ag-44 nanocluster.
Although atomically precise metalloid nanoclusters (NCs) of identical size with distinctly different molecular structures are highly desirable to understand the structural effects on the optical and photophysical properties, their synthesis remains highly challenging. Herein, we employed phosphine and thiol capping ligands featuring appropriate steric effects and synthesized a charge-neutral Ag NC with the formula Ag-44(EBT)(26)(TPP)(4) (EBT: 2-ethylbenzenethiolate; TPP: triphenylphosphine). The single-crystal X-ray structure reveals that this NC has a hollow metal core of Ag-12@Ag-20 and a metal-ligand shell of Ag-12(EBT)(26)(TPP)(4). The presence of mixed ligands and long V-shaped metal-ligand motifs on this NC has resulted in an enhancement of the NIR-II photoluminescence quantum yield by >25-fold compared to an all-thiolate-stabilized anionic [Ag-44(SR)(30)](4-) NC (SR: thiolate). Time-dependent density-functional calculations show that our Ag-44 NC is an 18-electron superatom with a modulated electronic structure as compared to the [Ag-44(SR)(30)](4-) anion, significantly influencing its optical properties.
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