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Probing the dynamics of plasmon-excited hexanethiol-capped gold nanoparticles by picosecond X-ray absorption spectroscopy

  • Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8% expansion of the Au–Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.

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Metadaten
Author:Flavio ZamponiGND, Thomas J. Penfold, Maarten Nachtegaal, Andrea Lübcke, Jochen Rittmann, Chris J. Milne, Majed Chergui, Jeroen A. van Bokhoven
DOI:https://doi.org/10.1039/c4cp03301a
ISSN:1463-9076 (print), 1463-9084 (online)
Parent Title (English):physical chemistry, chemical physics : PCCP
Document Type:Article
Language:English
Date of first Publication:2014/09/18
Year of Completion:2014
Publishing Institution:Universität Potsdam
Release Date:2015/03/26
Tag:TiO2 nanoparticles; diimine-complexes; electron-transfer; excitation; nanoclusters; reactivity; supported gold; surface; visible-light; water
Volume:2014
Issue:16
First Page:23157
Last Page:23163
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften
Peer Review:Referiert
Publication Way:Open Access
Grantor:RSC
Licence (English):License LogoCreative Commons - Attribution 3.0 unported
Notes extern:Zweitveröffentlichung als Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe ; 176