journal article·2022-06-14Open access

Fe3–xInSnxO6 (x = 0, 0.25, or 0.5): A Family of Corundum Derivatives with Sn-Induced Polarization and Above Room Temperature Antiferromagnetic Ordering

Corey E. Frank, Emma E. McCabe, Fabio Orlandi, Pascal Manuel, Xiaoyan Tan, Zheng Deng, Changqing Jin, Mark Croft, Thomas Emge, Shukai Yu, Huaiyu Wang, Venkatraman Gopalan, Saul Lapidus, MeiXia Wu, Man-Rong Li, Juliane Gross, Paul Burger, Aleksandra Mielewczyk-Gryń, Tomasz Klimczuk, Weiwei Xie, David Walker, Martha Greenblatt

Chemistry of Materials· Volume 34· Issue 11

Abstract

Three new double corundum derivative compounds, Fe3–xInSnxO6 (x = 0. 0.25, or 0.5), were synthesized at high pressure and temperature (6 GPa and 1400–1450 °C). All of the compounds order antiferromagnetically well above room temperature (TN = 608, 532, and 432 K for x = 0, 0.25, and 0.5, respectively). The x = 0 phase crystallizes as centrosymmetric R3̅c, but the inclusion of closed-shell d10 Sn4+ induces x = 0.25 and 0.5 to crystallize as noncentrosymmetric R3c. Microprobe measurements indicate that for x = 0.25 and 0.5, the substitution of Sn4+ is not offset by vacancies, which implies the presence of Fe2+, as corroborated by X-ray absorption near-edge spectroscopy and single-crystal X-ray structure refinements. Neutron powder diffraction experiments on x = 0.5 indicate that these compounds are canted A-type antiferromagnets that, like Fe2O3 and InFeO3, consist of ferromagnetic layers that stack antiferromagnetically with a single magnetic transition. Weak ferromagnetic interactions persist to very high temperatures. Temperature-dependent second harmonic generation (SHG) measurements on x = 0.25 and 0.5 show a SHG response with ferroelectric-like hysteretic maxima that correspond with the respective magnetic transitions, which suggest coupling of the magnetic and polarization order. These new compounds provide more information about fine-tuning the electronic, magnetic, and structural properties of corundum-derived mutlferroics in the search for tunable high-temperature magnetoelectric materials.
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Research context

OpenAlex topics: Multiferroics and related materials · Advanced Condensed Matter Physics · Magnetic and transport properties of perovskites and related materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, Piscataway, New Jersey 08854, United States

Department of Physics, Durham University, South Road, Durham DH1 3LE, United Kingdom

ISIS Facility, STFC, Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire OX11 0QX, United Kingdom

Department of Chemistry and Biochemistry, George Mason University, Fairfax, Virginia 22030, United States

Institute of Physics, School of Physics, University of Chinese Academy of Sciences, P.O. Box 603, Beijing 100190, P. R. China

Department of Physics and Astronomy, Rutgers, The State University of New Jersey, Piscataway, New Jersey 08854, United States

Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China

Department of Earth and Planetary Sciences, Rutgers, The State University of New Jersey, Piscataway, New Jersey 08854, United States

Faculty of Applied Physics and Mathematics, Gdansk University of Technology, ul. Narutowicza 11/12, 80-233 Gdańsk, Poland

Advanced Materials Centre, Gdansk University of Technology, ul. Narutowicza 11/12, 80-233 Gdańsk, Poland

Lamont Doherty Earth Observatory, Columbia University, Palisades, New York 10964, United States

Funding

Basic Energy Sciences · National Natural Science Foundation of China · Division of Materials Research

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