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Photoinduced anisotropic distortion as the electron trapping site of tungsten trioxide by ultrafast W L 1 -edge X-ray absorption spectroscopy with full potential multiple scattering calculations

Akihiro Koide 1, 2 Yohei Uemura 2, 3 Daiki Kido 4 Yuki Wakisaka 4 Satoru Takakusagi 4 Bunsho Ohtani 4 Yasuhiro Niwa 5 Shunsuke Nozawa 5 Kohei Ichiyanagi 5 Ryo Fukaya 5 Shin-Ichi Adachi 5 Tetsuo Katayama 6 Tadashi Togashi 6 Shigeki Owada 7 Makina Yabashi 7 Yusaku Yamamoto 8 Misaki Katayama 8 Keisuke Hatada 9 Toshihiko Yokoyama 2 Kiyotaka Asakura 4
1 IPR - Institut de Physique de Rennes
2 Institute for Molecular Science
3 Utrecht University [Utrecht]
4 Hokkaido University [Sapporo, Japan]
5 High energy accelerator research organization - KEK
6 JASRI - Japan Synchrotron Radiation Research Institute
7 RIKEN - RIKEN - Institute of Physical and Chemical Research [Japon]
8 Ritsumeikan University
9 University of Toyama
Abstract : Understanding the excited state of photocatalysts is significant to improve their activity for water splitting reaction. X-ray absorption fine structure (XAFS) spectroscopy in X-ray free electron lasers (XFEL) is a powerful method to address dynamic changes in electronic states and structures of photocatalysts in the excited state in ultrafast short time scales. The ultrafast atomic-scale local structural change in photoexcited WO3 was observed by W L1 edge XAFS spectroscopy using an XFEL. An anisotropic local distortion around the W atom could reproduce well the spectral features at a delay time of 100 ps after photoexcitation based on full potential multiple scattering calculations. The distortion involved the movement of W to shrink the shortest W–O bonds and elongate the longest one. The movement of the W atom could be explained by the filling of the dxy and dzx orbitals, which were originally located at the bottom of the conduction band with photoexcited electrons.
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https://hal-univ-rennes1.archives-ouvertes.fr/hal-02280133
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Submitted on : Monday, September 9, 2019 - 4:17:51 PM
Last modification on : Tuesday, June 16, 2020 - 3:44:02 PM
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Akihiro Koide, Yohei Uemura, Daiki Kido, Yuki Wakisaka, Satoru Takakusagi, et al.. Photoinduced anisotropic distortion as the electron trapping site of tungsten trioxide by ultrafast W L 1 -edge X-ray absorption spectroscopy with full potential multiple scattering calculations. Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2020, 22 (5), pp.2615-2621. ⟨10.1039/C9CP01332F⟩. ⟨hal-02280133⟩

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