Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction
Abstract
Co4Ta2O9 exhibits a three-dimensional magnetic lattice based on the buckled honeycomb motif. It shows unusual magnetoelectric effects, including the sign change and nonlinearity. These effects cannot be understood without the detailed knowledge of the magnetic structure. Herein, we report neutron diffraction and direction-dependent magnetic susceptibility measurements on Co4Ta2O9 single crystals. In this work, below 20.3 K, we find a long-range antiferromagnetic order in the alternating buckled and flat honeycomb layers of Co2+ ions stacked along the c axis. Within experimental accuracy, the magnetic moments lie in the ab plane. They form a canted antiferromagnetic structure with a tilt angle of ~14° at 15 K in the buckled layers, while the magnetic moments in each flat layer are collinear. This is directly evidenced by a finite (0, 0, 3) magnetic Bragg peak intensity, which would be absent in the collinear magnetic order. The magnetic space group is C2/c'. It is different from the previously reported C2/c' group, also found in the isostructural Co4Nb2O9. The revised magnetic structure successfully explains the major features of the magnetoelectric tensor of Co4Ta2O9 within the framework of the spin-flop model.
- Authors:
-
- Rutgers Univ., Piscataway, NJ (United States); Max Planck Institute for Solid State Research, Stuttgart (Germany)
- Yonsei Univ., Seoul (Korea, Republic of)
- Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab. (RAL)
- Rutgers Univ., Piscataway, NJ (United States); Ningbo University, Zhejiang (China)
- Max Planck Institute for Solid State Research, Stuttgart (Germany)
- Max Planck Institute for Intelligent Systems, Stuttgart (Germany)
- Rutgers Univ., Piscataway, NJ (United States)
- Publication Date:
- Research Org.:
- Rutgers Univ., Piscataway, NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF); China Scholarship Council (CSC); National Research Foundation of Korea (NRF)
- OSTI Identifier:
- 1849750
- Grant/Contract Number:
- FG02-07ER46382; DMR-1609935; NRF-2017R1A5A1014862; NRF-2018R1C1B6006859; NRF-2019R1A2C2002601
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 102; Journal Issue: 21; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Materials Science; Physics
Citation Formats
Choi, Sungkyun, Oh, Dong Gun, Gutmann, Matthias J., Pan, Shangke, Kim, Gideok, Son, Kwanghyo, Kim, Jaewook, Lee, Nara, Cheong, Sang-Wook, Choi, Young Jai, and Kiryukhin, Valery. Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction. United States: N. p., 2020.
Web. doi:10.1103/physrevb.102.214404.
Choi, Sungkyun, Oh, Dong Gun, Gutmann, Matthias J., Pan, Shangke, Kim, Gideok, Son, Kwanghyo, Kim, Jaewook, Lee, Nara, Cheong, Sang-Wook, Choi, Young Jai, & Kiryukhin, Valery. Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction. United States. https://doi.org/10.1103/physrevb.102.214404
Choi, Sungkyun, Oh, Dong Gun, Gutmann, Matthias J., Pan, Shangke, Kim, Gideok, Son, Kwanghyo, Kim, Jaewook, Lee, Nara, Cheong, Sang-Wook, Choi, Young Jai, and Kiryukhin, Valery. Wed .
"Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction". United States. https://doi.org/10.1103/physrevb.102.214404. https://www.osti.gov/servlets/purl/1849750.
@article{osti_1849750,
title = {Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction},
author = {Choi, Sungkyun and Oh, Dong Gun and Gutmann, Matthias J. and Pan, Shangke and Kim, Gideok and Son, Kwanghyo and Kim, Jaewook and Lee, Nara and Cheong, Sang-Wook and Choi, Young Jai and Kiryukhin, Valery},
abstractNote = {Co4Ta2O9 exhibits a three-dimensional magnetic lattice based on the buckled honeycomb motif. It shows unusual magnetoelectric effects, including the sign change and nonlinearity. These effects cannot be understood without the detailed knowledge of the magnetic structure. Herein, we report neutron diffraction and direction-dependent magnetic susceptibility measurements on Co4Ta2O9 single crystals. In this work, below 20.3 K, we find a long-range antiferromagnetic order in the alternating buckled and flat honeycomb layers of Co2+ ions stacked along the c axis. Within experimental accuracy, the magnetic moments lie in the ab plane. They form a canted antiferromagnetic structure with a tilt angle of ~14° at 15 K in the buckled layers, while the magnetic moments in each flat layer are collinear. This is directly evidenced by a finite (0, 0, 3) magnetic Bragg peak intensity, which would be absent in the collinear magnetic order. The magnetic space group is C2/c'. It is different from the previously reported C2/c' group, also found in the isostructural Co4Nb2O9. The revised magnetic structure successfully explains the major features of the magnetoelectric tensor of Co4Ta2O9 within the framework of the spin-flop model.},
doi = {10.1103/physrevb.102.214404},
journal = {Physical Review. B},
number = 21,
volume = 102,
place = {United States},
year = {Wed Dec 02 00:00:00 EST 2020},
month = {Wed Dec 02 00:00:00 EST 2020}
}
Works referenced in this record:
Trompe L’oeil Ferromagnetism
journal, June 2020
- Cheong, Sang-Wook
- npj Quantum Materials, Vol. 5, Issue 1
A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics
journal, January 1958
- Dzyaloshinsky, I.
- Journal of Physics and Chemistry of Solids, Vol. 4, Issue 4
Etude de niobates et tantalates de metaux de transition bivalents
journal, December 1961
- Bertaut, E. F.; Corliss, L.; Forrat, F.
- Journal of Physics and Chemistry of Solids, Vol. 21, Issue 3-4
Magnetoelectric coupling in the honeycomb antiferromagnet
journal, February 2016
- Khanh, N. D.; Abe, N.; Sagayama, H.
- Physical Review B, Vol. 93, Issue 7
Nature of magnetoelectric coupling in corundum antiferromagnet Co4Ta2O9
journal, April 2019
- Chaudhary, S.; Srivastava, P.; Kaushik, S. D.
- Journal of Magnetism and Magnetic Materials, Vol. 475
Type-II multiferroism and linear magnetoelectric coupling in the honeycomb antiferromagnet
journal, September 2018
- Maignan, Antoine; Martin, Christine
- Physical Review Materials, Vol. 2, Issue 9
: A magnetoelectric antiferromagnet
journal, April 2018
- Maignan, Antoine; Martin, Christine
- Physical Review B, Vol. 97, Issue 16
Advances in magnetoelectric multiferroics
journal, February 2019
- Spaldin, N. A.; Ramesh, R.
- Nature Materials, Vol. 18, Issue 3
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
Manipulation of electric polarization with rotating magnetic field in a honeycomb antiferromagnet
journal, September 2017
- Khanh, N. D.; Abe, N.; Kimura, S.
- Physical Review B, Vol. 96, Issue 9
Manipulating the magnetoelectric effect: Essence learned from
journal, January 2018
- Yanagi, Yuki; Hayami, Satoru; Kusunose, Hiroaki
- Physical Review B, Vol. 97, Issue 2
Symmetry Analysis of Magnetoelectric Effects in Honeycomb Antiferromagnet Co 4 Nb 2 O 9
journal, September 2019
- Matsumoto, Masashige; Koga, Mikito
- Journal of the Physical Society of Japan, Vol. 88, Issue 9
Theory of magnetoelectric response in Co4Nb2O9
journal, May 2018
- Yanagi, Yuki; Hayami, Satoru; Kusunose, Hiroaki
- Physica B: Condensed Matter, Vol. 536
Low-temperature crystal and magnetic structures of the magnetoelectric material
journal, September 2019
- Jana, Rajesh; Sheptyakov, Denis; Ma, Xiaoyan
- Physical Review B, Vol. 100, Issue 9
Origin of magnetoelectric effect in and : The lessons learned from the comparison of first-principles-based theoretical models and experimental data
journal, September 2016
- Solovyev, I. V.; Kolodiazhnyi, T. V.
- Physical Review B, Vol. 94, Issue 9
Large spin-driven dielectric response and magnetoelectric coupling in the buckled honeycomb
journal, August 2020
- Ding, Lei; Lee, Minseong; Choi, Eun Sang
- Physical Review Materials, Vol. 4, Issue 8
Spin dynamics and magnetoelectric coupling mechanism of
journal, February 2018
- Deng, Guochu; Cao, Yiming; Ren, Wei
- Physical Review B, Vol. 97, Issue 8
Highly nonlinear magnetoelectric effect in buckled-honeycomb antiferromagnetic Co4Ta2O9
journal, July 2020
- Lee, Nara; Oh, Dong Gun; Choi, Sungkyun
- Scientific Reports, Vol. 10, Issue 1
Anisotropic magnetodielectric coupling in antiferromagnet Co 4 Nb 2 O 9
journal, March 2019
- Khanh, N. D.; Abe, N.; Matsuura, K.
- Applied Physics Letters, Vol. 114, Issue 10
Extinction within the limit of validity of the Darwin transfer equations. III. Non-spherical crystals and anisotropy of extinction
journal, July 1975
- Becker, P. J.; Coppens, P.
- Acta Crystallographica Section A, Vol. 31, Issue 4
Multiferroics: a magnetic twist for ferroelectricity
journal, January 2007
- Cheong, Sang-Wook; Mostovoy, Maxim
- Nature Materials, Vol. 6, Issue 1
Anisotropic Superexchange Interaction and Weak Ferromagnetism
journal, October 1960
- Moriya, Tôru
- Physical Review, Vol. 120, Issue 1
The analytical calculation of absorption in multifaceted crystals
journal, November 1995
- Clark, R. C.; Reid, J. S.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 51, Issue 6
Crystallographic Computing System JANA2006: General features
journal, January 2014
- Petříček, Václav; Dušek, Michal; Palatinus, Lukáš
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 229, Issue 5
Extinction within the limit of validity of the Darwin transfer equations. II. Refinement of extinction in spherical crystals of SrF 2 and LiF
journal, March 1974
- Becker, P. J.; Coppens, P.
- Acta Crystallographica Section A, Vol. 30, Issue 2
Coupled magnetic and ferroelectric states in the distorted honeycomb system
journal, July 2018
- Panja, Soumendra Nath; Harnagea, Luminita; Kumar, Jitender
- Physical Review B, Vol. 98, Issue 2