A Polar Magnetic and Insulating Double Corundum Oxide: Mn2MnSbO6with Ordered Mn(II) and Mn(III) Ions

Hai L. Feng; Chang Jong Kang; Bongjae Kim; Kyoo Kim; Mark Croft; Sizhan Liu; Trevor A. Tyson; Eli Stavitski; Rui Zu; Venkatraman Gopalan; Saul H. Lapidus; Corey E. Frank; Youguo Shi; David Walker; Martha Greenblatt

doi:10.1021/acs.chemmater.1c02046

A Polar Magnetic and Insulating Double Corundum Oxide: Mn₂MnSbO₆with Ordered Mn(II) and Mn(III) Ions

Hai L. Feng, Chang Jong Kang, Bongjae Kim, Kyoo Kim, Mark Croft, Sizhan Liu, Trevor A. Tyson, Eli Stavitski, Rui Zu, Venkatraman Gopalan, Saul H. Lapidus, Corey E. Frank, Youguo Shi, David Walker, Martha Greenblatt

Physics

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Abstract

A new magnetic insulator Mn2MnSbO6 with a polar crystal structure and an ordered Mn2+ and Mn3+ arrangement was synthesized under a high pressure of 7.5 GPa and 1300 °C. The crystal structure of Mn2MnSbO6, investigated by synchrotron powder X-ray diffraction, was found to be isomorphous with that of Ni3TeO6-type, space group R3. The non-centrosymmetric structure was confirmed by the second-harmonic generation measurements. The X-ray absorption near-edge spectroscopy measurement confirmed the nominal oxidation states of Mn2+2Mn3+SbO6. Magnetic measurements indicate that Mn2MnSbO6 orders antiferromagnetically below 44 K and undergoes a field-induced spin-flop transition at 5 K. First-principles calculations indicate an antiferromagnetic ground state with up/up/up/down/down/down (uuuddd) spin configuration of the six crystallographically unique Mn ions in the c-axis doubled magnetic structure. The density functional theory calculations also substantiate the experimentally observed charge ordering of the Mn2+/Mn3+ ions and the insulating behavior due to a bandgap of 0.52 eV. To the best of our knowledge, this is the first double corundum oxide containing Jahn-Teller active Mn3+ ions.

Original language	English (US)
Pages (from-to)	6522-6529
Number of pages	8
Journal	Chemistry of Materials
Volume	33
Issue number	16
DOIs	https://doi.org/10.1021/acs.chemmater.1c02046
State	Published - Aug 24 2021

All Science Journal Classification (ASJC) codes

General Chemistry
General Chemical Engineering
Materials Chemistry

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Feng, H. L., Kang, C. J., Kim, B., Kim, K., Croft, M., Liu, S., Tyson, T. A., Stavitski, E., Zu, R., Gopalan, V., Lapidus, S. H., Frank, C. E., Shi, Y., Walker, D., & Greenblatt, M. (2021). A Polar Magnetic and Insulating Double Corundum Oxide: Mn₂MnSbO₆with Ordered Mn(II) and Mn(III) Ions. Chemistry of Materials, 33(16), 6522-6529. https://doi.org/10.1021/acs.chemmater.1c02046

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title = "A Polar Magnetic and Insulating Double Corundum Oxide: Mn2MnSbO6with Ordered Mn(II) and Mn(III) Ions",

abstract = "A new magnetic insulator Mn2MnSbO6 with a polar crystal structure and an ordered Mn2+ and Mn3+ arrangement was synthesized under a high pressure of 7.5 GPa and 1300 °C. The crystal structure of Mn2MnSbO6, investigated by synchrotron powder X-ray diffraction, was found to be isomorphous with that of Ni3TeO6-type, space group R3. The non-centrosymmetric structure was confirmed by the second-harmonic generation measurements. The X-ray absorption near-edge spectroscopy measurement confirmed the nominal oxidation states of Mn2+2Mn3+SbO6. Magnetic measurements indicate that Mn2MnSbO6 orders antiferromagnetically below 44 K and undergoes a field-induced spin-flop transition at 5 K. First-principles calculations indicate an antiferromagnetic ground state with up/up/up/down/down/down (uuuddd) spin configuration of the six crystallographically unique Mn ions in the c-axis doubled magnetic structure. The density functional theory calculations also substantiate the experimentally observed charge ordering of the Mn2+/Mn3+ ions and the insulating behavior due to a bandgap of 0.52 eV. To the best of our knowledge, this is the first double corundum oxide containing Jahn-Teller active Mn3+ ions.",

author = "Feng, {Hai L.} and Kang, {Chang Jong} and Bongjae Kim and Kyoo Kim and Mark Croft and Sizhan Liu and Tyson, {Trevor A.} and Eli Stavitski and Rui Zu and Venkatraman Gopalan and Lapidus, {Saul H.} and Frank, {Corey E.} and Youguo Shi and David Walker and Martha Greenblatt",

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doi = "10.1021/acs.chemmater.1c02046",

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T1 - A Polar Magnetic and Insulating Double Corundum Oxide

T2 - Mn2MnSbO6with Ordered Mn(II) and Mn(III) Ions

AU - Feng, Hai L.

AU - Kang, Chang Jong

AU - Kim, Bongjae

AU - Kim, Kyoo

AU - Croft, Mark

AU - Liu, Sizhan

AU - Tyson, Trevor A.

AU - Stavitski, Eli

AU - Zu, Rui

AU - Gopalan, Venkatraman

AU - Lapidus, Saul H.

AU - Frank, Corey E.

AU - Shi, Youguo

AU - Walker, David

AU - Greenblatt, Martha

PY - 2021/8/24

Y1 - 2021/8/24

N2 - A new magnetic insulator Mn2MnSbO6 with a polar crystal structure and an ordered Mn2+ and Mn3+ arrangement was synthesized under a high pressure of 7.5 GPa and 1300 °C. The crystal structure of Mn2MnSbO6, investigated by synchrotron powder X-ray diffraction, was found to be isomorphous with that of Ni3TeO6-type, space group R3. The non-centrosymmetric structure was confirmed by the second-harmonic generation measurements. The X-ray absorption near-edge spectroscopy measurement confirmed the nominal oxidation states of Mn2+2Mn3+SbO6. Magnetic measurements indicate that Mn2MnSbO6 orders antiferromagnetically below 44 K and undergoes a field-induced spin-flop transition at 5 K. First-principles calculations indicate an antiferromagnetic ground state with up/up/up/down/down/down (uuuddd) spin configuration of the six crystallographically unique Mn ions in the c-axis doubled magnetic structure. The density functional theory calculations also substantiate the experimentally observed charge ordering of the Mn2+/Mn3+ ions and the insulating behavior due to a bandgap of 0.52 eV. To the best of our knowledge, this is the first double corundum oxide containing Jahn-Teller active Mn3+ ions.

AB - A new magnetic insulator Mn2MnSbO6 with a polar crystal structure and an ordered Mn2+ and Mn3+ arrangement was synthesized under a high pressure of 7.5 GPa and 1300 °C. The crystal structure of Mn2MnSbO6, investigated by synchrotron powder X-ray diffraction, was found to be isomorphous with that of Ni3TeO6-type, space group R3. The non-centrosymmetric structure was confirmed by the second-harmonic generation measurements. The X-ray absorption near-edge spectroscopy measurement confirmed the nominal oxidation states of Mn2+2Mn3+SbO6. Magnetic measurements indicate that Mn2MnSbO6 orders antiferromagnetically below 44 K and undergoes a field-induced spin-flop transition at 5 K. First-principles calculations indicate an antiferromagnetic ground state with up/up/up/down/down/down (uuuddd) spin configuration of the six crystallographically unique Mn ions in the c-axis doubled magnetic structure. The density functional theory calculations also substantiate the experimentally observed charge ordering of the Mn2+/Mn3+ ions and the insulating behavior due to a bandgap of 0.52 eV. To the best of our knowledge, this is the first double corundum oxide containing Jahn-Teller active Mn3+ ions.

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JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 16

ER -

A Polar Magnetic and Insulating Double Corundum Oxide: Mn₂MnSbO₆with Ordered Mn(II) and Mn(III) Ions

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