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    Enhanced Negative Thermal Expansion Induced by Simultaneous Charge Transfer and Polar–Nonpolar Transitions
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    • Takumi Nishikubo*
      Takumi Nishikubo
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
      *[email protected]
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    • Yuki Sakai
      Yuki Sakai
      Kanagawa Institute of Industrial Science and Technology, 705-1 Shimoimaizumi, Ebina, Kanagawa 243-0435, Japan
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
      More by Yuki Sakai
    • Kengo Oka
      Kengo Oka
      Department of Applied Chemistry, Faculty of Science and Engineering, Kindai University, 3-4-1 Kowakae, Higashiosaka, Osaka 577-8502, Japan
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      Orcidhttp://orcid.org/0000-0002-1800-8575
    • Tetsu Watanuki
      Tetsu Watanuki
      Synchrotron Radiation Research Center, National Institutes for Quantum and Radiological Science and Technology, 1-1-1 Kouto, Sayo, Hyogo 679-5148, Japan
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    • Akihiko Machida
      Akihiko Machida
      Synchrotron Radiation Research Center, National Institutes for Quantum and Radiological Science and Technology, 1-1-1 Kouto, Sayo, Hyogo 679-5148, Japan
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    • Masaichiro Mizumaki
      Masaichiro Mizumaki
      Japan Synchrotron Radiation Research Institute, SPring-8, 1-1-1 Kouto, Sayo, Hyogo 679-5198, Japan
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    • Koki Maebayashi
      Koki Maebayashi
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
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    • Takashi Imai
      Takashi Imai
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
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    • Takahiro Ogata
      Takahiro Ogata
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
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    • Keisuke Yokoyama
      Keisuke Yokoyama
      Department of Chemistry, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro, Tokyo 152-8551, Japan
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    • Yoichi Okimoto
      Yoichi Okimoto
      Department of Chemistry, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro, Tokyo 152-8551, Japan
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    • Shin-ya Koshihara
      Shin-ya Koshihara
      Department of Chemistry, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro, Tokyo 152-8551, Japan
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    • Hajime Hojo
      Hajime Hojo
      Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University, 6-1 Kasuga-koen, Kasuga, Fukuoka 816-8580, Japan
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    • Takashi Mizokawa
      Takashi Mizokawa
      Department of Applied Physics, School of Advanced Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku, Tokyo 169-8555, Japan
      More by Takashi Mizokawa
      Orcidhttp://orcid.org/0000-0002-7682-2348
    • Masaki Azuma*
      Masaki Azuma
      Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
      Kanagawa Institute of Industrial Science and Technology, 705-1 Shimoimaizumi, Ebina, Kanagawa 243-0435, Japan
      *[email protected]
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      Orcidhttp://orcid.org/0000-0002-8378-321X
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2019, 141, 49, 19397–19403
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.9b10336
    Published November 18, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    Negative thermal expansion (NTE) induced by simultaneous mechanisms, that is, charge transfer and polar–nonpolar transitions, was observed for the first time in BiNi1–xFexO3 (0.25 ≤ x ≤ 0.5). The low-temperature phase was found to have a polar structure (space group of R3c) with a Bi3+0.5(1+x)Bi5+0.5(1–x)Ni2+1–xFe3+xO3 charge distribution and short-range ordering of Bi3+ and Bi5+. The volume reduction upon heating that was induced by charge transfer between Bi5+ and Ni2+ decreased with increasing x because of the reduction in the amount of Ni2+. Simultaneous polar–nonpolar transition also contributed to NTE, and a composition-independent enhanced volume reduction of ∼2% was observed.

    Copyright © 2019 American Chemical Society

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    • Rietveld refinement result for BiNi0.7Fe0.3O3 using a cubic (Pm-3m) structure; observed SXRD pattern and simulated peak position of R3 structure for BiNi0.7Fe0.3O3; temperature dependence of SXRD patterns for the samples with 0.6 ≤ x ≤ 0.9; temperature dependence of the pseudo cubic unit cell volume for BiNi0.3Fe0.7O3; structural parameters of BiNi0.7Fe0.3O3 obtained by Rietveld analysis carried out assuming a cubic Pm-3m structure; structural parameters of x = 0.4 and x = 0.5 samples (PDF)

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    Cite this: J. Am. Chem. Soc. 2019, 141, 49, 19397–19403
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.9b10336
    Published November 18, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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