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Photoinduced Charge Carrier Dynamics and Electron Injection Efficiencies in Au Nanoparticle-Sensitized TiO2 Determined with Picosecond Time-Resolved X-ray Photoelectron Spectroscopy

  • Mario Borgwardt
    Mario Borgwardt
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  • Johannes Mahl
    Johannes Mahl
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  • Friedrich Roth
    Friedrich Roth
    Institute of Experimental Physics, TU Bergakademie Freiberg, D-09599 Freiberg, Germany
  • Lukas Wenthaus
    Lukas Wenthaus
    Deutsches Elektronen Synchrotron/DESY, D-22607 Hamburg, Germany
  • Felix Brauße
    Felix Brauße
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  • Monika Blum
    Monika Blum
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    Chemical Sciences Division and Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    More by Monika Blum
  • Klaus Schwarzburg
    Klaus Schwarzburg
    Institute for Solar Fuels, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 14109 Berlin, Germany
  • Guiji Liu
    Guiji Liu
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, California 94720, United States
    More by Guiji Liu
  • Francesca M. Toma
    Francesca M. Toma
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, California 94720, United States
  • , and 
  • Oliver Gessner*
    Oliver Gessner
    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    *[email protected]
Cite this: J. Phys. Chem. Lett. 2020, 11, 14, 5476–5481
Publication Date (Web):June 16, 2020
https://doi.org/10.1021/acs.jpclett.0c00825
Copyright © 2020 American Chemical Society
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Abstract

Progress in the development of plasmon-enabled light-harvesting technologies requires a better understanding of their fundamental operating principles and current limitations. Here, we employ picosecond time-resolved X-ray photoemission spectroscopy to investigate photoinduced electron transfer in a plasmonic model system composed of 20 nm sized gold nanoparticles (NPs) attached to a nanoporous film of TiO2. The measurement provides direct, quantitative access to transient local charge distributions from the perspectives of the electron donor (AuNP) and the electron acceptor (TiO2). On average, approximately two electrons are injected per NP, corresponding to an electron injection yield per absorbed photon of 0.1%. Back electron transfer from the perspective of the electron donor is dominated by a fast recombination channel proceeding on a time scale of 60 ± 10 ps and a minor contribution that is completed after ∼1 ns. The findings provide a detailed picture of photoinduced charge carrier generation in this NP–semiconductor junction, with important implications for understanding achievable overall photon-to-charge conversion efficiencies.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c00825.

  • Sample preparation, time-resolved XPS experiment and reproducibility, UV–vis absorption spectra, SEM results, control experiment with Al2O3 substrate, Rayleigh stability limit and total static potential energy, fluence dependence of Au 4f line shift, and photoresponse at the Ti 2p edge (PDF)

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