Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand

Schwanen, Valérie; Remacle, Francoise

doi:10.1021/acs.nanolett.7b02568

Title: Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand

Journal Article · Mon Aug 14 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b02568· OSTI ID:1375260

Schwanen, Valérie ^[1];

^[1]

Theoretical Physical Chemistry, UR MOLSYS, University of Liège, B4000 Liège, Belgium

Because the development of attopulses, charge migration induced by short optical pulses has been extensively investigated. We report a computational purely electronic dynamical study of ultrafast few femtoseconds (fs) charge transfer and charge migration in realistic passivated stoichiometric Au11 and Au20 gold nanoclusters functionalized by a bipyridine ligand. We show that a net significant amount of electronic charge (0.1 to 0.4 |e| where |e| is the electron charge) is permanently transferred from the bipyridine chromophore to the gold cluster during the short 5–6 fs UV–vis strong pulse. This electron transfer to the metallic core is induced by the optical excitation of electronic states with a partial charge transfer character involving the chromophore before the onset of nuclei motion. In addition, the photoexcitation by the strong fs pulse builds a nonequilibrium electronic density that beats between the chromophore and the metallic core around the average of the transferred value. Modular systems made of a donor chromophore that can be photoexcited in the UV–vis range coupled to an efficient acceptor that could trap the charge are of interest for applications to nanodevices. Our study provides understanding on the very early, purely electronic dynamics built by the fs optical excitation and the initial charge separation step.

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Research Organization:: Wayne State Univ., Detroit, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Fonds National de la Recherche Scientifique (FNRS), Belgium

Grant/Contract Number:: SC0012628

OSTI ID:: 1375260

Alternate ID(s):: OSTI ID: 1473868; OSTI ID: 1507545

Journal Information:: Nano Letters, Journal Name: Nano Letters Vol. 17 Journal Issue: 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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Title: Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand

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