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

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 Au 11 and Au 20 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. Here, our study provides understanding on the very early, purely electronic dynamics built by the fs optical excitationmore » and the initial charge separation step.« less
Authors:
 [1] ; ORCiD logo [1]
  1. Univ. of Liège, Liège (Belgium). Theoretical Physical Chemistry
Publication Date:
Grant/Contract Number:
SC0012628
Type:
Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 9; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Wayne State Univ., Detroit, MI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Fonds National de la Recherche Scientifique (FNRS), Belgium
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; attochemistry; charge migration; Charge transfer; electronic quantum dynamics; gold cluster
OSTI Identifier:
1375260
Alternate Identifier(s):
OSTI ID: 1473868

Schwanen, Valérie, and Remacle, Francoise. Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand. United States: N. p., Web. doi:10.1021/acs.nanolett.7b02568.
Schwanen, Valérie, & Remacle, Francoise. Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand. United States. doi:10.1021/acs.nanolett.7b02568.
Schwanen, Valérie, and Remacle, Francoise. 2017. "Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand". United States. doi:10.1021/acs.nanolett.7b02568.
@article{osti_1375260,
title = {Photoinduced Ultrafast Charge Transfer and Charge Migration in Small Gold Clusters Passivated by a Chromophoric Ligand},
author = {Schwanen, Valérie and Remacle, Francoise},
abstractNote = {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. Here, our study provides understanding on the very early, purely electronic dynamics built by the fs optical excitation and the initial charge separation step.},
doi = {10.1021/acs.nanolett.7b02568},
journal = {Nano Letters},
number = 9,
volume = 17,
place = {United States},
year = {2017},
month = {8}
}