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Large Polarization Switching and High-Temperature Magnetoelectric Coupling in Multiferroic GaFeO3 Systems

  • Hui Wang
    Hui Wang
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    More by Hui Wang
  • Yang Zhang
    Yang Zhang
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    More by Yang Zhang
  • Koki Tachiyama
    Koki Tachiyama
    Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan
  • Zhaoyang Xia
    Zhaoyang Xia
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100049, China
    More by Zhaoyang Xia
  • Jinghong Fang
    Jinghong Fang
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100049, China
  • Qin Li
    Qin Li
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    More by Qin Li
  • Guofeng Cheng
    Guofeng Cheng
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
  • Yun Shi
    Yun Shi
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    More by Yun Shi
  • Jianding Yu*
    Jianding Yu
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Science, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100049, China
    *Email: [email protected]
    More by Jianding Yu
  • Tsukasa Katayama
    Tsukasa Katayama
    Department of Chemistry, The University of Tokyo, Bunkyo-ku, Tokyo 113-0033, Japan
  • Shintaro Yasui
    Shintaro Yasui
    Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan
    Laboratory for Advanced Nuclear Energy, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8550, Japan
  • , and 
  • Mitsuru Itoh
    Mitsuru Itoh
    Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan
    Research Institute for Advanced Electronics and Photonics (RIAEP), National Institute of Advanced Industrial Science and Technology Central-2, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan
    More by Mitsuru Itoh
Cite this: Inorg. Chem. 2021, 60, 1, 225–230
Publication Date (Web):December 15, 2020
https://doi.org/10.1021/acs.inorgchem.0c02855
Copyright © 2020 American Chemical Society

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    Abstract

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    GaFeO3-type iron oxides are promising multiferroics due to the coexistence of large spontaneous magnetization and polarization near room temperature. However, the high leakage current and difficulties associated with synthesizing single crystals make it difficult to achieve two important features in the system: a large ferroelectric polarization switching and magnetoelectric coupling at a high-temperature region. Herein, we report successful achievement of these features by preparing high-quality Sc-doped GaFeO3 single crystals (ScxGa1–x/2Fe1–x/2O3 with x = 0–0.3) using the floating zone method. The x ≥ 0.05 crystals exhibit a leakage current 104 times lower than the x = 0 crystals, highlighting the importance of Sc doping. Because of the reduced leakage current, the Sc-doped crystals exhibit large ferroelectric polarization switching along the c-axis with a remanent polarization of 22–25 μC/cm2, which is close to the theoretically predicted polarization value of 25–28 μC/cm2. In addition, the Sc-doped crystals exhibit ferrimagnetism with magnetic anisotropy along the a-axis. Furthermore, a magnetic-field-induced modulation of polarization is observed in the x = 0.15 crystal even at a relatively high temperature, i.e., 100 K.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.0c02855.

    • Single-crystal and Laue photographs, Arrhenius plots, polarization and current versus electric field curves, and element analysis by ICP (PDF)

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    Cited By

    This article is cited by 7 publications.

    1. Yang Zhang, Hui Wang, Koki Tachiyama, Tsukasa Katayama, Yinghao Zhu, Si Wu, Hai-Feng Li, Jinghong Fang, Qin Li, Yun Shi, Ling Wang, Zhengqian Fu, Fangfang Xu, Jianding Yu, Shintaro Yasui, Mitsuru Itoh. Single-Crystal Synthesis of ε-Fe2O3-Type Oxides Exhibiting Room-Temperature Ferrimagnetism and Ferroelectric Polarization. Crystal Growth & Design 2021, 21 (9) , 4904-4908. https://doi.org/10.1021/acs.cgd.1c00310
    2. Maria Biernacka, Paweł Butkiewicz, Konrad J. Kapcia, Wojciech Olszewski, Dariusz Satuła, Marek Szafrański, Marcin Wojtyniak, Krzysztof R. Szymański. Electrical polarization switching in bulk single-crystal GaFe O 3 . Physical Review B 2023, 108 (19) https://doi.org/10.1103/PhysRevB.108.195101
    3. Jeong Kyu Kim, Bongjae Kim, Dong-Hwan Kim, Kyoo Kim, Arata Tanaka, Younghak Kim, Sang-Wook Cheong, Kyung-Tae Ko, Jae-Hoon Park. Electronic origin of ferroelectricity in multiferroic Lu 0.5 Sc 0.5 FeO 3 . Physical Review B 2023, 108 (15) https://doi.org/10.1103/PhysRevB.108.155152
    4. Ling Wang, Tsukasa Katayama, Chaoyue Wang, Qin Li, Yun Shi, Yuqiang Fang, Fuqiang Huang, Yinghao Zhu, Hai-feng Li, Shintaro Yasui, Xintang Huang, Jianding Yu. Enhancement of room-temperature magnetization in GaFeO3-type single crystals by Al and Sc doping. AIP Advances 2022, 12 (6) https://doi.org/10.1063/5.0088234
    5. Maria Biernacka, Marek Szafrański, Katarzyna Rećko, Wojciech Olszewski, Dariusz Satuła, Paweł Butkiewicz, Krzysztof R. Szymański. Heat capacity anomaly near magnetic phase transition in GaFeO3. Journal of Magnetism and Magnetic Materials 2022, 548 , 168978. https://doi.org/10.1016/j.jmmm.2021.168978
    6. Mitsuru Itoh, Yosuke Hamasaki, Hiroshi Takashima, Rie Yokoi, Ayako Taguchi, Hiroki Moriwake. Chemical design of a new displacive-type ferroelectric. Dalton Transactions 2022, 51 (7) , 2610-2630. https://doi.org/10.1039/D1DT03693A
    7. Yuying Yang, Zhiyan Chen, Xiangqian Lu, Xiaotao Hao, Wei Qin. All organic multiferroic magnetoelectric complexes with strong interfacial spin-dipole interaction. npj Flexible Electronics 2021, 5 (1) https://doi.org/10.1038/s41528-021-00120-0

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