Controlling inversion disorder in a stoichiometric spinel magnet

Margarita G. Dronova; Feng Ye; Scott E. Cooper; Anjana Krishnadas; Christina M. Hoffmann; Yuita Fujisawa; Yoshinori Okada; Daniel I. Khomskii; Yejun Feng

doi:10.1073/pnas.2208748119

Controlling inversion disorder in a stoichiometric spinel magnet

Margarita G. Dronova, Feng Ye, Scott E. Cooper, Anjana Krishnadas, Christina M. Hoffmann, Yuita Fujisawa, Yoshinori Okada, Daniel I. Khomskii, Yejun Feng

Single Crystal Diffraction

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

In the study of frustrated quantum magnets, it is essential to be able to control the nature and degree of site disorder during the growth process, as many measurement techniques are incapable of distinguishing between site disorder and frustration-induced spin disorder. Pyrochlore-structured spinel oxides can serve as model systems of geometrically frustrated three-dimensional quantum magnets; however, the nature of the magnetism in one well-studied spinel, ZnFe₂O₄, remains unclear. Here, we demonstrate simultaneous control of both stoichiometry and inversion disorder in the growth of ZnFe₂O₄ single crystals, directly yielding a revised understanding of both the collective spin behavior and lattice symmetry. Crystals grown in the stoichiometric limit with minimal site inversion disorder contravene all the previously suggested exotic spin phases in ZnFe₂O₄. Furthermore, the structure is confirmed on the F 43m space group with broken inversion symmetry that induces antiferroelectricity. The effective tuning of magnetic behavior by site disorder in the presence of robust antiferroelectricity makes ZnFe₂O₄ of special interest to multiferroic devices.

Original language	English
Article number	e2208748119
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	119
Issue number	43
DOIs	https://doi.org/10.1073/pnas.2208748119
State	Published - Oct 25 2022

Funding

ACKNOWLEDGMENTS. We acknowledge insightful discussion with Yishu Wang. We also thank N. Ishizu and the Mechanical Engineering and Microfabrication Support Section of the Okinawa Institute of Science and Technology for technical support and the usage of shared equipment. Y. Feng acknowledges financial support from the Okinawa Institute of Science and Technology Graduate University, with subsidy funding from the Cabinet Office, Government of Japan. D.I.K. was supported by the German Research Foundation (Deutsche Forschungsgemeinschaft) under Project 277146847-CRC1238. A portion of this research used resources at the Spallation Neutron Source, a US Department of Energy Office of Science User Facility operated by the Oak Ridge National Laboratory. We acknowledge insightful discussion with Yishu Wang. We also thank N. Ishizu and the Mechanical Engineering and Microfabrication Support Section of the Okinawa Institute of Science and Technology for technical support and the usage of shared equipment. Y. Feng acknowledges financial support from the Okinawa Institute of Science and Technology Graduate University, with subsidy funding from the Cabinet Office, Government of Japan. D.I.K. was supported by the German Research Foundation (Deutsche Forschungsgemeinschaft) under Project 277146847-CRC1238. A portion of this research used resources at the Spallation Neutron Source, a US Department of Energy Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
Office of Science
Oak Ridge National Laboratory
Deutsche Forschungsgemeinschaft	277146847-CRC1238
Cabinet Office, Government of Japan
Okinawa Institute of Science and Technology Graduate University

Keywords

antiferroelectricity
antiferromagnetic spinel
inversion disorder
neutron magnetic diffuse scattering
single-crystal growth

Access to Document

10.1073/pnas.2208748119

Cite this

@article{681fb7d88fb940dc90bd9afbdf6af9f5,

title = "Controlling inversion disorder in a stoichiometric spinel magnet",

abstract = "In the study of frustrated quantum magnets, it is essential to be able to control the nature and degree of site disorder during the growth process, as many measurement techniques are incapable of distinguishing between site disorder and frustration-induced spin disorder. Pyrochlore-structured spinel oxides can serve as model systems of geometrically frustrated three-dimensional quantum magnets; however, the nature of the magnetism in one well-studied spinel, ZnFe2O4, remains unclear. Here, we demonstrate simultaneous control of both stoichiometry and inversion disorder in the growth of ZnFe2O4 single crystals, directly yielding a revised understanding of both the collective spin behavior and lattice symmetry. Crystals grown in the stoichiometric limit with minimal site inversion disorder contravene all the previously suggested exotic spin phases in ZnFe2O4. Furthermore, the structure is confirmed on the F 43m space group with broken inversion symmetry that induces antiferroelectricity. The effective tuning of magnetic behavior by site disorder in the presence of robust antiferroelectricity makes ZnFe2O4 of special interest to multiferroic devices.",

keywords = "antiferroelectricity, antiferromagnetic spinel, inversion disorder, neutron magnetic diffuse scattering, single-crystal growth",

author = "Dronova, {Margarita G.} and Feng Ye and Cooper, {Scott E.} and Anjana Krishnadas and Hoffmann, {Christina M.} and Yuita Fujisawa and Yoshinori Okada and Khomskii, {Daniel I.} and Yejun Feng",

note = "Publisher Copyright: Copyright {\textcopyright} 2022 the Author(s). Published by PNAS.",

year = "2022",

month = oct,

day = "25",

doi = "10.1073/pnas.2208748119",

language = "English",

volume = "119",

journal = "Proceedings of the National Academy of Sciences of the United States of America",

issn = "0027-8424",

publisher = "National Academy of Sciences",

number = "43",

}

TY - JOUR

T1 - Controlling inversion disorder in a stoichiometric spinel magnet

AU - Dronova, Margarita G.

AU - Ye, Feng

AU - Cooper, Scott E.

AU - Krishnadas, Anjana

AU - Hoffmann, Christina M.

AU - Fujisawa, Yuita

AU - Okada, Yoshinori

AU - Khomskii, Daniel I.

AU - Feng, Yejun

PY - 2022/10/25

Y1 - 2022/10/25

N2 - In the study of frustrated quantum magnets, it is essential to be able to control the nature and degree of site disorder during the growth process, as many measurement techniques are incapable of distinguishing between site disorder and frustration-induced spin disorder. Pyrochlore-structured spinel oxides can serve as model systems of geometrically frustrated three-dimensional quantum magnets; however, the nature of the magnetism in one well-studied spinel, ZnFe2O4, remains unclear. Here, we demonstrate simultaneous control of both stoichiometry and inversion disorder in the growth of ZnFe2O4 single crystals, directly yielding a revised understanding of both the collective spin behavior and lattice symmetry. Crystals grown in the stoichiometric limit with minimal site inversion disorder contravene all the previously suggested exotic spin phases in ZnFe2O4. Furthermore, the structure is confirmed on the F 43m space group with broken inversion symmetry that induces antiferroelectricity. The effective tuning of magnetic behavior by site disorder in the presence of robust antiferroelectricity makes ZnFe2O4 of special interest to multiferroic devices.

AB - In the study of frustrated quantum magnets, it is essential to be able to control the nature and degree of site disorder during the growth process, as many measurement techniques are incapable of distinguishing between site disorder and frustration-induced spin disorder. Pyrochlore-structured spinel oxides can serve as model systems of geometrically frustrated three-dimensional quantum magnets; however, the nature of the magnetism in one well-studied spinel, ZnFe2O4, remains unclear. Here, we demonstrate simultaneous control of both stoichiometry and inversion disorder in the growth of ZnFe2O4 single crystals, directly yielding a revised understanding of both the collective spin behavior and lattice symmetry. Crystals grown in the stoichiometric limit with minimal site inversion disorder contravene all the previously suggested exotic spin phases in ZnFe2O4. Furthermore, the structure is confirmed on the F 43m space group with broken inversion symmetry that induces antiferroelectricity. The effective tuning of magnetic behavior by site disorder in the presence of robust antiferroelectricity makes ZnFe2O4 of special interest to multiferroic devices.

KW - antiferroelectricity

KW - antiferromagnetic spinel

KW - inversion disorder

KW - neutron magnetic diffuse scattering

KW - single-crystal growth

UR - http://www.scopus.com/inward/record.url?scp=85140186775&partnerID=8YFLogxK

U2 - 10.1073/pnas.2208748119

DO - 10.1073/pnas.2208748119

M3 - Article

C2 - 36256823

AN - SCOPUS:85140186775

SN - 0027-8424

VL - 119

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

IS - 43

M1 - e2208748119

ER -

Controlling inversion disorder in a stoichiometric spinel magnet

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this