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Electron localization in rod-shaped triicosahedral gold nanocluster [electronic resource].

Published:
Washington, D.C. : United States. Dept. of Energy. Office of Basic Energy Sciences, 2017.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description:
pages E4,697-E4,705 : digital, PDF file
Additional Creators:
Brookhaven National Laboratory, United States. Department of Energy. Office of Basic Energy Sciences, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary:
Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. There is little known about the carrier dynamics in these nanoclusters, which limit their energy-related applications. We reported the observation of exciton localization in triicosahedral Au37 nanoclusters (0.5 nm in diameter and 1.6 nm in length) by measuring femtosecond and nanosecond carrier dynamics. Upon photoexcitation to S1 electronic state, electrons in Au37 undergo ~100-ps localization from the two vertexes of three icosahedrons to one vertex, forming a long-lived S1* state. Such phenomenon is not observed in Au25 (dimer) and Au13 (monomer) consisting of two and one icosahedrons, respectively. We have further observed temperature dependence on the localization process, which proves it is thermally driven. Two excited-state vibration modes with frequencies of 20 and 70 cm-1 observed in the kinetic traces are assigned to the axial and radial breathing modes, respectively. The electron localization is ascribed to the structural distortion of Au37 in the excited state induced by the strong coherent vibrations. The electron localization phenomenon we observed provides unique physical insight into one-dimensional gold nanoclusters and other nanostructures, which will advance their applications in solar-energy storage and conversion.
Report Numbers:
E 1.99:bnl--114330-2017-ja
bnl--114330-2017-ja
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Note:
Published through SciTech Connect.
05/30/2017.
"bnl--114330-2017-ja"
"KC0403020"
Proceedings of the National Academy of Sciences of the United States of America 114 24 ISSN 0027-8424 AM
Meng Zhou; Renxi Jin; Matthew Y. Sfeir; Yuxiang Chen; Yongbo Song; Rongchao Jin.
Funding Information:
SC0012704
AC02-98CH10886
View MARC record | catkey: 24056399