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Revealing the Role of Hydrogen in Electron-Doping Mottronics for Strongly Correlated Vanadium Dioxide

  • Xuanchi Zhou
    Xuanchi Zhou
    School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083 China
    More by Xuanchi Zhou
  • Haifan Li
    Haifan Li
    School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083 China
    More by Haifan Li
  • Fanqi Meng
    Fanqi Meng
    School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
    More by Fanqi Meng
  • Wei Mao*
    Wei Mao
    Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
    School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-0032, Japan
    *Email: [email protected]
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  • Jiaou Wang
    Jiaou Wang
    Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
    More by Jiaou Wang
  • Yong Jiang*
    Yong Jiang
    School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083 China
    *Email: [email protected]
    More by Yong Jiang
  • Katsuyuki Fukutani
    Katsuyuki Fukutani
    Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
  • Markus Wilde
    Markus Wilde
    Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
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  • Bunshi Fugetsu
    Bunshi Fugetsu
    Institute for Future Initiatives, The University of Tokyo, Bunkyo-ku, Tokyo 113-0032, Japan
  • Ichiro Sakata
    Ichiro Sakata
    School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-0032, Japan
    Institute for Future Initiatives, The University of Tokyo, Bunkyo-ku, Tokyo 113-0032, Japan
  • Nuofu Chen
    Nuofu Chen
    School of Renewable Energy, North China Electric Power University, Beijing 102206, China
    More by Nuofu Chen
  • , and 
  • Jikun Chen*
    Jikun Chen
    School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083 China
    *Email: [email protected]
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Cite this: J. Phys. Chem. Lett. 2022, 13, 34, 8078–8085
Publication Date (Web):August 23, 2022
https://doi.org/10.1021/acs.jpclett.2c02001
Copyright © 2022 American Chemical Society

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    Abstract

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    Hydrogen-associated electron-doping Mottronics for d-band correlated oxides (e.g., VO2) opens up a new paradigm to regulate the electronic functionality via directly manipulating the orbital configuration and occupancy. Nevertheless, the role of hydrogen in the Mottronic transition of VO2 is yet unclear because opposite orbital reconfigurations toward either the metallic or highly insulating states were both reported. Herein, we demonstrate the root cause for such hydrogen-induced multiple electronic phase transitions by 1H quantification using nuclear reaction analysis. A low hydrogenation temperature is demonstrated to be vital in achieving a large hydrogen concentration (nH ≈ 1022 cm–3) that further enhances the t2g orbital occupancy to trigger electron localizations. In contrast, elevating the hydrogenation temperatures surprisingly reduces nH to ∼1021 cm–3 but forms more stable metallic H0.06VO2. This leads to the recognition of a weaker hydrogen interaction that triggers electron localization within VO2 via Mottronically enhancing the orbital occupancies.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.2c02001.

    • Hydrogenation procedure, atomic force macroscopy surface morphology, X-ray diffraction (XRD) patterns, the derivation of Ea and TMott, and additional X-ray photoelectron spectroscopy results (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 4 publications.

    1. Alexandre Pofelski, Haili Jia, Sunbin Deng, Haoming Yu, Tae Joon Park, Sukriti Manna, Maria K.Y. Chan, Subramanian K. R. S. Sankaranarayanan, Shriram Ramanathan, Yimei Zhu. Subnanometer Scale Mapping of Hydrogen Doping in Vanadium Dioxide. Nano Letters 2024, 24 (6) , 1974-1980. https://doi.org/10.1021/acs.nanolett.3c04411
    2. Muhammad Umer Fayaz, Qian Wang, Shixuan Liang, Lei Han, Feng Pan, Cheng Song. Protonation-Induced Colossal Lattice Expansion in La2/3Sr1/3MnO3. ACS Applied Materials & Interfaces 2023, 15 (49) , 57388-57396. https://doi.org/10.1021/acsami.3c14270
    3. Xuanchi Zhou, Yuchen Cui, Yanlong Shang, Haifan Li, Jiaou Wang, Ye Meng, Xiaoguang Xu, Yong Jiang, Nuofu Chen, Jikun Chen. Non-equilibrium Spark Plasma Reactive Doping Enables Highly Adjustable Metal-to-Insulator Transitions and Improved Mechanical Stability for VO2. The Journal of Physical Chemistry C 2023, 127 (5) , 2639-2647. https://doi.org/10.1021/acs.jpcc.2c07631
    4. Benjamin M. Lefler, William M. Postiglione, Chris Leighton, Steven J. May. Voltage Control of Patterned Metal/Insulator Properties in Oxide/Oxyfluoride Lateral Perovskite Heterostructures via Ion Gel Gating. Advanced Functional Materials 2022, 32 (49) , 2208434. https://doi.org/10.1002/adfm.202208434

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