MnFe0.5Ru0.5O3: an above-room-temperature antiferromagnetic semiconductor

Xiaoyan Tan; Emma E. McCabe; Fabio Orlandi; Pascal Manuel; Maria Batuk; Joke Hadermann; Zheng Deng; Changqing Jin; Israel Nowik; Rolfe Herber; Carlo U. Segre; Sizhan Liu; Mark Croft; Chang-Jong Kang; Saul Lapidus; Corey E. Frank; Haricharan Padmanabhan; Venkatraman Gopalan; Meixia Wu; Man-Rong Li; Gabriel Kotliar; David Walker; Martha Greenblatt

doi:10.1039/C8TC05059G

MnFe_0.5Ru_0.5O₃: an above-room-temperature antiferromagnetic semiconductor†

Xiaoyan Tan,

‡^a Emma E. McCabe,

^b Fabio Orlandi,

^c Pascal Manuel,^c Maria Batuk,^d Joke Hadermann,

^d Zheng Deng,^e Changqing Jin,^e Israel Nowik,^f Rolfe Herber,

^f Carlo U. Segre,

^g Sizhan Liu,^h Mark Croft,ⁱ Chang-Jong Kang,

ⁱ Saul Lapidus,^j Corey E. Frank,

^a Haricharan Padmanabhan,^k Venkatraman Gopalan,^k Meixia Wu,^l Man-Rong Li,

^l Gabriel Kotliar,ⁱ David Walker^m and Martha Greenblatt

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry and Chemical Biology Rutgers, The State University of New Jersey, Piscataway, New Jersey, USA
E-mail: greenbla@chem.rutgers.edu

^b School of Physical Sciences, University of Kent, Canterbury, Kent, UK

^c ISIS Facility, STFC, Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire, UK

^d EMAT, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, Belgium

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

^f Racah Institute of Physics, The Hebrew University, Jerusalem, Israel

^g Department of Physics & CSRRI, Illinois Institute of Technology, Chicago, Illinois, USA

^h Department of Physics, New Jersey Institute of Technology, Newark, New Jersey, USA

ⁱ Department of Physics and Astronomy, Rutgers, The State University of New Jersey, Piscataway, New Jersey, USA

^j Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois, USA

^k Department of Materials Science and Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, USA

^l Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, Sun Yat-Sen University, Guangzhou, P. R. China

^m Lamont Doherty Earth Observatory, Columbia University, Palisades, New York, USA

Abstract

A transition-metal-only MnFe_0.5Ru_0.5O₃ polycrystalline oxide was prepared by a reaction of starting materials MnO, MnO₂, Fe₂O₃, RuO₂ at 6 GPa and 1873 K for 30 minutes. A combination of X-ray and neutron powder diffraction refinements indicated that MnFe_0.5Ru_0.5O₃ adopts the corundum (α-Fe₂O₃) structure type with space group R [3 with combining macron] c, in which all metal ions are disordered. The centrosymmetric nature of the MnFe_0.5Ru_0.5O₃ structure is corroborated by transmission electron microscopy, lack of optical second harmonic generation, X-ray absorption near edge spectroscopy, and Mössbauer spectroscopy. X-ray absorption near edge spectroscopy of MnFe_0.5Ru_0.5O₃ showed the oxidation states of Mn, Fe, and Ru to be 2+/3+, 3+, and ∼4+, respectively. Resistivity measurements revealed that MnFe_0.5Ru_0.5O₃ is a semiconductor. Magnetic measurements and magnetic structure refinements indicated that MnFe_0.5Ru_0.5O₃ orders antiferromagnetically around 400 K, with magnetic moments slightly canted away from the c axis. ⁵⁷Fe Mössbauer confirmed the magnetic ordering and Fe³⁺ (S = 5/2) magnetic hyperfine splitting. First principles calculations are provided to understand the electronic structure more thoroughly. A comparison of synthesis and properties of MnFe_0.5Ru_0.5O₃ and related corundum Mn₂BB′O₆ derivatives is discussed.

This article is part of the themed collection: 2019 Journal of Materials Chemistry C HOT Papers

Journal of Materials Chemistry C

MnFe_0.5Ru_0.5O₃: an above-room-temperature antiferromagnetic semiconductor†

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MnFe_0.5Ru_0.5O₃: an above-room-temperature antiferromagnetic semiconductor

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Journal of Materials Chemistry C