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

Sang Han Park, Abhishek Katoch, Keun Hwa Chae, Sanjeev Gautam, Piter Miedema, Sang Wan Cho, Minseok Kim, Ru-Pan Wang, Masoud Lazemi, Frank Groot () and Soonnam Kwon ()
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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
Masoud Lazemi: Utrecht University
Frank Groot: Utrecht University
Soonnam Kwon: Pohang Accelerator Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-30336-1

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