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Origin of Unexpected Ir3+ in a Superconducting Candidate Sr2IrO4 System Analyzed by Photoelectron Holography
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    Origin of Unexpected Ir3+ in a Superconducting Candidate Sr2IrO4 System Analyzed by Photoelectron Holography
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    • Rie Horie*
      Rie Horie
      Research Institute for Interdisciplinary Science (RIIS), Okayama University, Okayama 700-8530, Japan
      *Email: [email protected]
      More by Rie Horie
    • Tomohiro Matsushita
      Tomohiro Matsushita
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Sota Kawamura
      Sota Kawamura
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Tsubasa Hase
      Tsubasa Hase
      Department of Precision Engineering, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
      More by Tsubasa Hase
    • Kazumasa Horigane
      Kazumasa Horigane
      Research Institute for Interdisciplinary Science (RIIS), Okayama University, Okayama 700-8530, Japan
    • Hiroki Momono
      Hiroki Momono
      National Institute of Technology, Yonago College, Yonago, Tottori 683-8502, Japan
    • Soichiro Takeuchi
      Soichiro Takeuchi
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Masaki Tanaka
      Masaki Tanaka
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Hiroto Tomita
      Hiroto Tomita
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Yusuke Hashimoto
      Yusuke Hashimoto
      Graduate School of Science and Technology, Nara Institute of Science and Technology, Ikoma, Nara 630-0192, Japan
    • Kaya Kobayashi
      Kaya Kobayashi
      Research Institute for Interdisciplinary Science (RIIS), Okayama University, Okayama 700-8530, Japan
      Graduate School of Natural Science and Technology, Okayama University, Okayama 700-8530, Japan
    • Yuichi Haruyama
      Yuichi Haruyama
      Laboratory of Advanced Science and Technology for Industry, University of Hyogo, Ako, Hyogo 678-1205, Japan
    • Hiroshi Daimon*
      Hiroshi Daimon
      Toyota Physical and Chemical Research Institute, Nagakute, Aichi 480-1192, Japan
      *Email: [email protected]
    • Yoshitada Morikawa
      Yoshitada Morikawa
      Department of Precision Engineering, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
    • Munetaka Taguchi
      Munetaka Taguchi
      Toshiba Nanoanalysis Corporation, Yokohama 235-8522, Japan
    • Jun Akimitsu
      Jun Akimitsu
      Research Institute for Interdisciplinary Science (RIIS), Okayama University, Okayama 700-8530, Japan
      More by Jun Akimitsu
    Other Access OptionsSupporting Information (1)

    Inorganic Chemistry

    Cite this: Inorg. Chem. 2023, 62, 28, 10897–10904
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    https://doi.org/10.1021/acs.inorgchem.2c03788
    Published June 2, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    The reason for the absence of superconductivity in Sr2IrO4 was estimated by photoelectron spectra and photoelectron holograms. The analysis of the La photoelectron hologram concluded that La atoms are substituted to Sr sites. Two O 1s peaks were observed and were identified as the oxygens in the IrO2 and SrO planes by photoelectron holography and density functional theory (DFT) calculations. In the Ir 4f spectrum of Sr2IrO4, an unexpected Ir3+ peak was observed as much as 50% of all of the Ir. The photoelectron hologram of Ir3+ showed a displacement of about 0.15 Å. This displacement is thought to be due to the oxygen vacancies in the IrO2 plane. These oxygen vacancies and the associated local displacement of the atoms might inhibit superconductivity in spite of sufficient electron doping.

    Copyright © 2023 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.inorgchem.2c03788.

    • Details of the DFT calculation method; details of the calculation of XPS core-level spectra; schematic diagram of the retarding field analyzer (RFA) (Figure S1); photoelectron spectra from Sr2IrO4 (Figure S2); comparison of experimental photoelectron holograms and simulations for Sr2IrO4 (Figure S3); three-dimensional atomic structure around the Ir3+ atom reconstructed by the holography method (Figure S4); and atomic structure around O vacancy (Figure S5) (PDF)

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    Cited By

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    This article is cited by 2 publications.

    1. Yusuke Hashimoto, Jun Mizuno, Hiroyuki Matsuda, Fumihiko Matsui, Tomohiro Matsushita. High-resolution electron energy analyzer with wide acceptance angle for hard X-ray photoelectron holography: integrating PESCATORA and retarding field analyzer. Japanese Journal of Applied Physics 2024, 63 (12) , 124001. https://doi.org/10.35848/1347-4065/ad9447
    2. Zhilai Yue, Keke Jiao, Weili Zhen, Huijie Hu, Rui Niu, Changjin Zhang. Electron Doping and Enhanced Conductivity in Vacuum Annealed Sr2-xLaxIrO4. Journal of Superconductivity and Novel Magnetism 2024, 37 (2) , 409-417. https://doi.org/10.1007/s10948-024-06696-8

    Inorganic Chemistry

    Cite this: Inorg. Chem. 2023, 62, 28, 10897–10904
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.2c03788
    Published June 2, 2023
    Copyright © 2023 American Chemical Society

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