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Direct and real-time observation of hole transport dynamics in anatase TiO2 using X-ray free-electron laser

Author

Listed:
  • Sang Han Park

    (Pohang Accelerator Laboratory)

  • Abhishek Katoch

    (Pohang Accelerator Laboratory)

  • Keun Hwa Chae

    (Korea Institute of Science and Technology)

  • Sanjeev Gautam

    (Dr S. S. Bhatnagar University Institute of Chemical Engineering & Technology, Panjab University)

  • Piter Miedema

    (European XFEL Gmbh)

  • Sang Wan Cho

    (Yonsei Univerity)

  • Minseok Kim

    (Pohang Accelerator Laboratory)

  • Ru-Pan Wang

    (Utrecht University
    University of Hamburg)

  • Masoud Lazemi

    (Utrecht University)

  • Frank Groot

    (Utrecht University)

  • Soonnam Kwon

    (Pohang Accelerator Laboratory)

Abstract

Carrier dynamics affects photocatalytic systems, but direct and real-time observations in an element-specific and energy-level-specific manner are challenging. In this study, we demonstrate that the dynamics of photo-generated holes in metal oxides can be directly probed by using femtosecond X-ray absorption spectroscopy at an X-ray free-electron laser. We identify the energy level and life time of holes with a long life time (230 pico-seconds) in nano-crystal materials. We also observe that trapped holes show an energy distribution in the bandgap region with a formation time of 0.3 pico-seconds and a decay time of 8.0 pico-seconds at room temperature. We corroborate the dynamics of the electrons by using X-ray absorption spectroscopy at the metal L-edges in a consistent explanation with that of the holes.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30336-1
    DOI: 10.1038/s41467-022-30336-1
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    References listed on IDEAS

    as
    1. 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.
    2. Hikmet Sezen & Honghui Shang & Fabian Bebensee & Chengwu Yang & Maria Buchholz & Alexei Nefedov & Stefan Heissler & Christian Carbogno & Matthias Scheffler & Patrick Rinke & Christof Wöll, 2015. "Correction: Corrigendum: Evidence for photogenerated intermediate hole polarons in ZnO," Nature Communications, Nature, vol. 6(1), pages 1-1, November.
    3. E. Baldini & L. Chiodo & A. Dominguez & M. Palummo & S. Moser & M. Yazdi-Rizi & G. Auböck & B.P.P. Mallett & H. Berger & A. Magrez & C. Bernhard & M. Grioni & A. Rubio & M. Chergui, 2017. "Strongly bound excitons in anatase TiO2 single crystals and nanoparticles," Nature Communications, Nature, vol. 8(1), pages 1-11, December.
    4. Hikmet Sezen & Honghui Shang & Fabian Bebensee & Chengwu Yang & Maria Buchholz & Alexei Nefedov & Stefan Heissler & Christian Carbogno & Matthias Scheffler & Patrick Rinke & Christof Wöll, 2015. "Evidence for photogenerated intermediate hole polarons in ZnO," Nature Communications, Nature, vol. 6(1), pages 1-5, November.
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