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, Mei Xia Wu, Man Rong Li, Juliane Gross, Paul Burger, Aleksandra Mielewczyk-Gryń, Tomasz Klimczuk, Weiwei XieDavid Walker, Martha Greenblatt

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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 R3¯ c, 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.

Original languageEnglish (US)
Pages (from-to)5020-5029
Number of pages10
JournalChemistry of Materials
Volume34
Issue number11
DOIs
StatePublished - Jun 14 2022

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Chemical Engineering
  • Materials Chemistry

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