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Fe3-xInSnxO6 (x = 0, 0.25, 0.5): A family of corundum derivatives with Sn-induced polarization and above room temperature antiferromagnetic ordering

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

Fe3-xInSnxO6 (x = 0, 0.25, 0.5): A family of corundum derivatives with Sn-induced polarization and above room temperature antiferromagnetic ordering Thumbnail


Authors

Corey E. Frank

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



Abstract

Three new double corundum derived compounds, Fe3-xInSnxO6, (x = 0. 0.25, 0.5) were synthesized at high pressure and temperature (6 GPa, 1400-1450 C) All the compounds order antiferromagnetically well above room temperature, TN = 608 K, 532K, and 432 K for x = 0, 0.25, 0.5, respectively. The x = 0 phase crystalizes as centrosymmetric R3c, but increasing the substitution 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, 0.5, the substitution of Sn4+ is not compensated for 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 which, 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 measurements on x = 0.25 and 0.5 show 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 on fine-tuning the electronic, magnetic and structural properties of corundum derived mutlferroics in the search for tunable high temperature magnetoelectric materials.

Journal Article Type Article
Acceptance Date May 19, 2022
Online Publication Date Jun 2, 2022
Publication Date Jun 14, 2022
Deposit Date May 20, 2022
Publicly Available Date Jun 2, 2023
Journal Chemistry of Materials
Print ISSN 0897-4756
Electronic ISSN 1520-5002
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 34
Issue 11
Pages 5020-5029
DOI https://doi.org/10.1021/acs.chemmater.2c00312
Public URL https://durham-repository.worktribe.com/output/1206693

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Copyright Statement
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.2c00312






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