期刊
ACS NANO
卷 15, 期 10, 页码 16095-16105出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c04759
关键词
gold nanoclusters; NIR emissions; structure-property relations; improvement of PL efficiency; high-pressure
类别
资金
- National Science Foundation (NSF) [DMR-2002936/2002891, ECCS-1542152]
- DOE [DE-AC02-06CH11357]
- Office of the Provost, the Office for Research, and Northwestern University Information Technology
Gold nanoclusters with near-infrared photoluminescence show potential for sensing and imaging in biomedical applications. The study focuses on two types of gold nanoclusters, Au-21(S-Adm)(15) and Au38S2(S-Adm)(20), and explores the mechanisms behind their improved quantum yields, large Stokes shifts, and long photoluminescence lifetimes. Results suggest that the surface lock rings play a key role in achieving high quantum yields in gold nanoclusters.
Gold nanoclusters with near-infrared (NIR) photoluminescence (PL) have great potential as sensing and imaging materials in biomedical and bioimaging applications. In this work, Au-21(S-Adm)(15) and Au38S2(S-Adm)(20) are used to unravel the underlying mechanisms for the improved quantum yields (QY), large Stokes shifts, and long PL lifetimes in gold nanoclusters. Both nanoclusters show decent PL QY. In particular, the Au38S2(S-Adm) 20 nanocluster shows a bright NIR PL at 900 nm with QY up to 15% in normal solvents (such as toluene) at ambient conditions. The relatively lower QY for Au-21(S-Adm)(15) (4%) compared to that of Au38S2(S-Adm)(20) is attributed to the lowest-lying excited state being symmetry-disallowed, as evidenced by the pressure-dependent antispectral shift of the absorption spectra compared to PL, yet Au-21(S-Adm)(15) maintains some emissive properties due to a nearby symmetry-allowed excited state. Furthermore, our results show that suppression of nonradiative decay due to the surface lock rings, which encircle the Au kernel and the surface lock atoms which bridge the fundamental Au kernel units (e.g., tetrahedra, icosahedra, etc.), is the key to obtaining high QYs in gold nanoclusters. The complicated excited-state processes and the small absorption coefficient of the band-edge transition lead to the large Stokes shifts and the long PL lifetimes that are widely observed in gold nanoclusters.
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