期刊
NANOSCALE
卷 13, 期 10, 页码 5300-5306出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0nr07624d
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资金
- National Natural Science Foundation of China [21722308, 22003072]
- Key Research Program of CAS Frontier Sciences (CAS) [QYZDBSSWSLH024]
- Beijing Natural Science Foundation [2192064]
- Frontier Cross Project of National Laboratory for Molecular Sciences [051Z011BZ3]
A highly stable Cu-doped undeca-gold cluster with a unique coordination structure was synthesized in this study. The nanocluster exhibits superatom stability and interesting optical properties, showing emissions in both ultraviolet-visible and near infrared regions with novel anti-Stokes up-conversion lasing characteristics.
We have synthesized single crystals of a highly stable Cu-doped undeca-gold cluster protected by both triphenylphosphine (PPh3) and 2-pyridinethiol (-SPy) ligands, formulated as [Au11Cu1(PPh3)(7)(SPy)(3)](+). This cluster (Au11Cu1 NCs for short) has a metallic core of C-3v Au@Au-10 with the Cu atom capped on one of the nine triangular facets and it is triply-coordinated to three N atoms of the SPy ligands of which the sulfur atom simultaneously binds to three adjacent Au atoms via singly-coordinated S-Au bonds, respectively. The other seven gold atoms form a crown structure by a link of three orthogons with common sides and are protected by seven PPh3 ligands. Besides the well-organized coordination, this Au11Cu1 nanocluster is demonstrated to exhibit superatom stability of the metallic core within 8 valence electrons (assuming that the 3 electrophilic-SPy ligands capture 3 electrons from the metal center). More interestingly, this Au11Cu1 nanocluster shows interesting emissions in both ultraviolet visible (UV-Vis) and near infrared (NIR) regions, and the emissions display novel anti-Stokes up-conversion lasing characteristics. TD-DFT calculated UV-vis and emission spectra well reproduce the experimental results, shedding light on the nature of excitation states and underlying mechanism of electronic transitions between diverse energy levels of such a monolayer-protected bimetallic cluster.
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