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Charge Separation, Band-Bending, and Recombination in WO3 Photoanodes

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    Charge Separation, Band-Bending, and Recombination in WO3 Photoanodes
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    • Sacha Corby
      Sacha Corby
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
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      Orcidhttp://orcid.org/0000-0001-7863-5426
    • Ernest Pastor
      Ernest Pastor
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
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    • Yifan Dong
      Yifan Dong
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
      More by Yifan Dong
    • Xijia Zheng
      Xijia Zheng
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
      More by Xijia Zheng
    • Laia Francàs
      Laia Francàs
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
      More by Laia Francàs
      Orcidhttp://orcid.org/0000-0001-9171-6247
    • Michael Sachs
      Michael Sachs
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
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      Orcidhttp://orcid.org/0000-0001-9775-9336
    • Shababa Selim
      Shababa Selim
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
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    • Andreas Kafizas
      Andreas Kafizas
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
      Grantham Institute for Climate Change, Imperial College London, South Kensington, London SW7 2AZ, United Kingdom
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      Orcidhttp://orcid.org/0000-0002-2282-4639
    • Artem A. Bakulin
      Artem A. Bakulin
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
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      Orcidhttp://orcid.org/0000-0002-3998-2000
    • James R. Durrant*
      James R. Durrant
      Department of Chemistry and Centre for Plastic Electronics, Imperial College London, White City Campus, London W12 0BZ, United Kingdom
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0001-8353-7345
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2019, 10, 18, 5395–5401
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    https://doi.org/10.1021/acs.jpclett.9b01935
    Published August 16, 2019
    Copyright © 2019 American Chemical Society
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    In metal oxide-based photoelectrochemical devices, the spatial separation of photogenerated electrons and holes is typically attributed to band-bending at the oxide/electrolyte interface. However, direct evidence of such band-bending impacting upon charge carrier lifetimes has been very limited to date. Herein we use ultrafast spectroscopy to track the rapid relaxation of holes in the space-charge layer and their recombination with trapped electrons in WO3 photoanodes. We observe that applied bias can significantly increase carrier lifetimes on all time scales from picoseconds to seconds and attribute this to enhanced band-bending correlated with changes in oxygen vacancy state occupancy. We show that analogous enhancements in carrier lifetimes can be obtained by changes in electrolyte composition, even in the absence of applied bias, highlighting routes to improve photoconversion yields/performance, through changes in band-bending. This study thus demonstrates the direct connection between carrier lifetime enhancement, increased band-bending, and oxygen vacancy defect state occupancy.

    Copyright © 2019 American Chemical Society

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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2019, 10, 18, 5395–5401
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.9b01935
    Published August 16, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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