Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction

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

doi:10.1103/physrevb.102.214404

Title: 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:

Choi, Sungkyun ^[1]; Oh, Dong Gun ^[2]; Gutmann, Matthias J. ^[3]; Pan, Shangke ^[4]; Kim, Gideok ^[5];

^[6];

^[7]; Lee, Nara ^[2]; Cheong, Sang-Wook ^[7]; Choi, Young Jai ^[2];

^[7]

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:: Wed Dec 02 00:00:00 EST 2020

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.

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                    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

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                    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.

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@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}

}

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Title: Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co4Ta2O9 determined by single-crystal neutron diffraction

Abstract

Citation Formats

Trompe L’oeil Ferromagnetism journal, June 2020

A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics journal, January 1958

Etude de niobates et tantalates de metaux de transition bivalents journal, December 1961

Magnetoelectric coupling in the honeycomb antiferromagnet Co 4 Nb 2 O 9 journal, February 2016

Nature of magnetoelectric coupling in corundum antiferromagnet Co4Ta2O9 journal, April 2019

Type-II multiferroism and linear magnetoelectric coupling in the honeycomb F e 4 T a 2 O 9 antiferromagnet journal, September 2018

Fe 4 Nb 2 O 9 : A magnetoelectric antiferromagnet journal, April 2018

Advances in magnetoelectric multiferroics journal, February 2019

Recent advances in magnetic structure determination by neutron powder diffraction journal, October 1993

Manipulation of electric polarization with rotating magnetic field in a honeycomb antiferromagnet Co 4 Nb 2 O 9 journal, September 2017

Manipulating the magnetoelectric effect: Essence learned from Co 4 Nb 2 O 9 journal, January 2018

Symmetry Analysis of Magnetoelectric Effects in Honeycomb Antiferromagnet Co 4 Nb 2 O 9 journal, September 2019

Theory of magnetoelectric response in Co4Nb2O9 journal, May 2018

Low-temperature crystal and magnetic structures of the magnetoelectric material F e 4 N b 2 O 9 journal, September 2019

Origin of magnetoelectric effect in Co 4 Nb 2 O 9 and Co 4 Ta 2 O 9 : The lessons learned from the comparison of first-principles-based theoretical models and experimental data journal, September 2016

Large spin-driven dielectric response and magnetoelectric coupling in the buckled honeycomb Fe 4 Nb 2 O 9 journal, August 2020

Spin dynamics and magnetoelectric coupling mechanism of C o 4 N b 2 O 9 journal, February 2018

Highly nonlinear magnetoelectric effect in buckled-honeycomb antiferromagnetic Co4Ta2O9 journal, July 2020

Anisotropic magnetodielectric coupling in antiferromagnet Co 4 Nb 2 O 9 journal, March 2019

Extinction within the limit of validity of the Darwin transfer equations. III. Non-spherical crystals and anisotropy of extinction journal, July 1975

Multiferroics: a magnetic twist for ferroelectricity journal, January 2007

Anisotropic Superexchange Interaction and Weak Ferromagnetism journal, October 1960

The analytical calculation of absorption in multifaceted crystals journal, November 1995

Crystallographic Computing System JANA2006: General features journal, January 2014

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

Coupled magnetic and ferroelectric states in the distorted honeycomb system Fe 4 Ta 2 O 9 journal, July 2018

Title: Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co₄Ta₂O₉ determined by single-crystal neutron diffraction

Trompe L’oeil Ferromagnetism
journal, June 2020

A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics
journal, January 1958

Etude de niobates et tantalates de metaux de transition bivalents
journal, December 1961

Magnetoelectric coupling in the honeycomb antiferromagnet ${Co}_{4} {Nb}_{2} O_{9}$
journal, February 2016

Nature of magnetoelectric coupling in corundum antiferromagnet Co4Ta2O9
journal, April 2019

Type-II multiferroism and linear magnetoelectric coupling in the honeycomb $F e_{4} T a_{2} O_{9}$ antiferromagnet
journal, September 2018

${Fe}_{4} {Nb}_{2} O_{9}$ : A magnetoelectric antiferromagnet
journal, April 2018

Advances in magnetoelectric multiferroics
journal, February 2019

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993

Manipulation of electric polarization with rotating magnetic field in a honeycomb antiferromagnet ${Co}_{4} {Nb}_{2} O_{9}$
journal, September 2017

Manipulating the magnetoelectric effect: Essence learned from ${Co}_{4} {Nb}_{2} O_{9}$
journal, January 2018

Symmetry Analysis of Magnetoelectric Effects in Honeycomb Antiferromagnet Co ₄ Nb ₂ O ₉
journal, September 2019

Theory of magnetoelectric response in Co4Nb2O9
journal, May 2018

Low-temperature crystal and magnetic structures of the magnetoelectric material $F e_{4} N b_{2} O_{9}$
journal, September 2019

Origin of magnetoelectric effect in ${Co}_{4} {Nb}_{2} O_{9}$ and ${Co}_{4} {Ta}_{2} O_{9}$ : The lessons learned from the comparison of first-principles-based theoretical models and experimental data
journal, September 2016

Large spin-driven dielectric response and magnetoelectric coupling in the buckled honeycomb ${Fe}_{4} {Nb}_{2} O_{9}$
journal, August 2020

Spin dynamics and magnetoelectric coupling mechanism of $C o_{4} N b_{2} O_{9}$
journal, February 2018

Highly nonlinear magnetoelectric effect in buckled-honeycomb antiferromagnetic Co4Ta2O9
journal, July 2020

Anisotropic magnetodielectric coupling in antiferromagnet Co ₄ Nb ₂ O ₉
journal, March 2019

Extinction within the limit of validity of the Darwin transfer equations. III. Non-spherical crystals and anisotropy of extinction
journal, July 1975

Multiferroics: a magnetic twist for ferroelectricity
journal, January 2007

Anisotropic Superexchange Interaction and Weak Ferromagnetism
journal, October 1960

The analytical calculation of absorption in multifaceted crystals
journal, November 1995

Crystallographic Computing System JANA2006: General features
journal, January 2014

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

Coupled magnetic and ferroelectric states in the distorted honeycomb system ${Fe}_{4} {Ta}_{2} O_{9}$
journal, July 2018