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Electronic structure transformation in small bare Au clusters as seen by x-ray photoelectron spectroscopy
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
Oulu Univ, Dept Phys Sci, Box 3000, FI-90014 Oulu, Finland..
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2017 (English)In: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 50, no 1, 015102Article in journal (Refereed) Published
Abstract [en]

Free bare gold clusters in the size range from few tens to few hundred atoms (<= 1 nm dimensions) have been produced in a beam, and the size-dependent development of their full valence band including the 5d and 6s parts has been mapped 'on the fly' by synchrotron-based photoelectron spectroscopy. The Au 4f core level has been also probed, and the cluster-specific Au 4f ionization energies have been used to estimate the cluster size. The recorded in the present work valence spectra of the small clusters are compared with the spectra of the large clusters (N similar to 10(3)) created by us using a magnetron-based gas aggregation source. The comparison shows a substantially narrower 5d valence band and the decrease in its splitting for gold clusters in the size range of few hundred atoms and below. Our DFT calculations involving the pseudopotential method show that the 5d band width of the ground state increases with the cluster size and by the size N = 20 becomes comparable with the experimental width of the valence photoelectron spectrum. Similar to the earlier observations on supported clusters we interpret our experimental and theoretical results as due to the undercoordination of a large fraction of atoms in the clusters with N similar to 10(2) and below. The consequences of such electronic structure of small gold clusters are discussed in connection with their specific physical and chemical properties related to nanoplasmonics and nanocatalysis.

Place, publisher, year, edition, pages
2017. Vol. 50, no 1, 015102
Keyword [en]
Au 5d valence band, Au 4f core level, free bare clusters, synchrotron radiation, x-ray photoelectron spectroscopy, size-dependent electronic structure
National Category
Condensed Matter Physics Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:uu:diva-316008DOI: 10.1088/1361-6455/50/1/015102ISI: 000391492400001OAI: oai:DiVA.org:uu-316008DiVA: diva2:1076981
Funder
Swedish Research CouncilGöran Gustafsson Foundation for promotion of scientific research at Uppala University and Royal Institute of TechnologyKnut and Alice Wallenberg FoundationThe Crafoord FoundationSwedish Foundation for Strategic Research
Available from: 2017-02-24 Created: 2017-02-24 Last updated: 2017-02-24Bibliographically approved

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Björneholm, Olle
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