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Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering
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    Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering
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    • Bijuan Chen*
      Bijuan Chen
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      *E-mail: [email protected]. (B.C.)
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    • Ekaterina M. Pärschke*
      Ekaterina M. Pärschke
      Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294, United States
      *E-mail: [email protected]. (E.M.P.)
    • Wei-Chih Chen
      Wei-Chih Chen
      Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294, United States
    • Brandon Scoggins
      Brandon Scoggins
      Department of Physics, University of North Georgia, Dahlonega, Georgia 30533, United States
    • Bing Li
      Bing Li
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      More by Bing Li
    • Mahalingam Balasubramanian
      Mahalingam Balasubramanian
      Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
    • Steve Heald
      Steve Heald
      Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
      More by Steve Heald
    • Jianbo Zhang
      Jianbo Zhang
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      More by Jianbo Zhang
    • Hongshan Deng
      Hongshan Deng
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
    • Raimundas Sereika
      Raimundas Sereika
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
    • Yesudhas Sorb
      Yesudhas Sorb
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
    • Xia Yin
      Xia Yin
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      More by Xia Yin
    • Yan Bi
      Yan Bi
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      More by Yan Bi
    • Ke Jin
      Ke Jin
      National Key Laboratory of Shock Wave and Detonation Physics, Institute of Fluid Physics, CAEP, Mianyang 621900, China
      More by Ke Jin
    • Qiang Wu
      Qiang Wu
      National Key Laboratory of Shock Wave and Detonation Physics, Institute of Fluid Physics, CAEP, Mianyang 621900, China
      More by Qiang Wu
    • Cheng-Chien Chen*
      Cheng-Chien Chen
      Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294, United States
      *E-mail: [email protected]. (C.-C.C.)
    • Yang Ding*
      Yang Ding
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      *E-mail: [email protected]. (Y.D.)
      More by Yang Ding
    • Ho-kwang Mao
      Ho-kwang Mao
      Center for High-Pressure Science & Technology Advanced Research, Beijing 100094, P.R. China
      Geophysical Laboratory, Carnegie Institution of Washington, Washington, D.C. 20015, United States
      More by Ho-kwang Mao
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2019, 10, 24, 7890–7897
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.9b02819
    Published December 9, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    Understanding the volume collapse phenomena in rare-earth materials remains an important challenge due to a lack of information on 4f electronic structures at different pressures. Here, we report the first high-pressure inelastic X-ray scattering measurement on elemental cerium (Ce) metal. By overcoming the ultralow signal issue in the X-ray measurement at the Ce N4,5-edge, we observe the changes of unoccupied 4f states across the volume collapse transition around 0.8 GPa. To help resolve the longstanding debate on the Anderson–Kondo and Mott–Hubbard models, we further compare the experiments with extended multiplet calculations that treat both screening channels on equal footing. The results indicate that a modest change in the 4f–5d Kondo coupling can well describe the spectral redistribution across the volume collapse, whereas the hybridization between neighboring atoms in the Hubbard model appears to play a minor role. Our study helps to constrain the theoretical models and opens a promising new route for systematic investigation of volume collapse phenomena in rare-earth materials.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.9b02819.

    • Experimental X-ray spectra collected using different gaskets, X-ray diffraction patterns of different cerium systems, and additional simulated X-ray spectra for the Kondo and Hubbard models (PDF)

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    This article is cited by 9 publications.

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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2019, 10, 24, 7890–7897
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.9b02819
    Published December 9, 2019
    Copyright © 2019 American Chemical Society

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