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Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy

Author

Listed:
  • Thomas J. Penfold

    (Newcastle University)

  • Jakub Szlachetko

    (Paul Scherrer Institut
    Polish Academy of Sciences)

  • Fabio G. Santomauro

    (FSB and Lausanne Centre for Ultrafast Science (LACUS))

  • Alexander Britz

    (European XFEL
    The Hamburg Centre for Ultrafast Imaging)

  • Wojciech Gawelda

    (European XFEL
    Faculty of Physics, Adam Mickiewicz University)

  • Gilles Doumy

    (Argonne National Laboratory)

  • Anne Marie March

    (Argonne National Laboratory)

  • Stephen H. Southworth

    (Argonne National Laboratory)

  • Jochen Rittmann

    (FSB and Lausanne Centre for Ultrafast Science (LACUS))

  • Rafael Abela

    (Paul Scherrer Institut)

  • Majed Chergui

    (FSB and Lausanne Centre for Ultrafast Science (LACUS))

  • Christopher J. Milne

    (Paul Scherrer Institut)

Abstract

Nanostructures of transition metal oxides, such as zinc oxide, have attracted considerable interest for solar-energy conversion and photocatalysis. Both applications are sensitive to the transport and trapping of photoexcited charge carriers. The probing of electron trapping has recently become possible using time-resolved element-sensitive methods, such as X-ray spectroscopy. However, valence-band-trapped holes have so far escaped observation. Herein we use X-ray absorption spectroscopy combined with a dispersive X-ray emission spectrometer to probe the charge carrier relaxation and trapping processes in zinc oxide nanoparticles after above band-gap photoexcitation. Our results, supported by simulations, demonstrate that within 80 ps, photoexcited holes are trapped at singly charged oxygen vacancies, which causes an outward displacement by ~15% of the four surrounding zinc atoms away from the doubly charged vacancy. This identification of the hole traps provides insight for future developments of transition metal oxide-based nanodevices.

Suggested Citation

  • Thomas J. Penfold & Jakub Szlachetko & Fabio G. Santomauro & Alexander Britz & Wojciech Gawelda & Gilles Doumy & Anne Marie March & Stephen H. Southworth & Jochen Rittmann & Rafael Abela & Majed Cherg, 2018. "Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-02870-4
    DOI: 10.1038/s41467-018-02870-4
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    Cited by:

    1. Zhi Chen & Jie Wang & Hongbo Wu & Jianming Yang & Yikai Wang & Jing Zhang & Qinye Bao & Ming Wang & Zaifei Ma & Wolfgang Tress & Zheng Tang, 2022. "A Transparent Electrode Based on Solution-Processed ZnO for Organic Optoelectronic Devices," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Sang Han Park & Abhishek Katoch & Keun Hwa Chae & Sanjeev Gautam & Piter Miedema & Sang Wan Cho & Minseok Kim & Ru-Pan Wang & Masoud Lazemi & Frank Groot & Soonnam Kwon, 2022. "Direct and real-time observation of hole transport dynamics in anatase TiO2 using X-ray free-electron laser," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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