DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice

Abstract

The standard approach to realize a spin-liquid state is through magnetically frustrated states, relying on ingredients such as the lattice geometry, dimensionality, and magnetic interaction type of the spins. While Heisenberg spins on a pyrochlore lattice with only antiferromagnetic nearest-neighbor interactions are theoretically proven disordered, spins in real systems generally include longer-range interactions. The spatial correlations at longer distances typically stabilize a long-range order rather than enhancing a spin-liquid state. Both states can, however, be destroyed by short-range static correlations introduced by chemical disorder. Here, using disorder-free specimens with a clear long-range antiferromagnetic order, we refine the spin structure of the Heisenberg spinel ZnFe2O4through neutron magnetic diffraction. The unique wave vector (1, 0, $$\frac{1}{2}$$) leads to a spin structure that can be viewed as alternatively stacked ferromagnetic and antiferromagnetic tetrahedra in a three-dimensional checkerboard form. Stable coexistence of these opposing types of clusters is enabled by the bipartite breathing pyrochlore crystal structure, leading to a second-order phase transition at 10 K. The diffraction intensity of ZnFe2O4 is an exact complement to the inelastic scattering intensity of several chromate spinel systems which are regarded as model classical spin liquids. Our results challenge this attribution, and suggest instead of the six-spin ring mode, spin excitations in chromate spinels are closely related to the (1, 0, $$\frac{1}{2}$$) type of spin order and the four-spin ferromagnetic cluster locally at one tetrahedron.

Authors:
 [1];  [2];  [3]; ORCiD logo [3]; ORCiD logo [4];  [1]
  1. Okinawa Institute of Science and Technology Graduate University (Japan)
  2. Czech Academy of Sciences (CAS), Prague (Czech Republic)
  3. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  4. California Institute of Technology (CalTech), Pasadena, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
2324011
Grant/Contract Number:  
AC05-00OR22725; FA9550-20-1-0263
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B
Additional Journal Information:
Journal Volume: 109; Journal Issue: 6; 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

Citation Formats

Dronova, Margarita G., Petříček, Václav, Morgan, Zachary, Ye, Feng, Silevitch, Daniel M., and Feng, Yejun. Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice. United States: N. p., 2024. Web. doi:10.1103/physrevb.109.064421.
Dronova, Margarita G., Petříček, Václav, Morgan, Zachary, Ye, Feng, Silevitch, Daniel M., & Feng, Yejun. Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice. United States. https://doi.org/10.1103/physrevb.109.064421
Dronova, Margarita G., Petříček, Václav, Morgan, Zachary, Ye, Feng, Silevitch, Daniel M., and Feng, Yejun. Fri . "Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice". United States. https://doi.org/10.1103/physrevb.109.064421. https://www.osti.gov/servlets/purl/2324011.
@article{osti_2324011,
title = {Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice},
author = {Dronova, Margarita G. and Petříček, Václav and Morgan, Zachary and Ye, Feng and Silevitch, Daniel M. and Feng, Yejun},
abstractNote = {The standard approach to realize a spin-liquid state is through magnetically frustrated states, relying on ingredients such as the lattice geometry, dimensionality, and magnetic interaction type of the spins. While Heisenberg spins on a pyrochlore lattice with only antiferromagnetic nearest-neighbor interactions are theoretically proven disordered, spins in real systems generally include longer-range interactions. The spatial correlations at longer distances typically stabilize a long-range order rather than enhancing a spin-liquid state. Both states can, however, be destroyed by short-range static correlations introduced by chemical disorder. Here, using disorder-free specimens with a clear long-range antiferromagnetic order, we refine the spin structure of the Heisenberg spinel ZnFe2O4through neutron magnetic diffraction. The unique wave vector (1, 0, $\frac{1}{2}$) leads to a spin structure that can be viewed as alternatively stacked ferromagnetic and antiferromagnetic tetrahedra in a three-dimensional checkerboard form. Stable coexistence of these opposing types of clusters is enabled by the bipartite breathing pyrochlore crystal structure, leading to a second-order phase transition at 10 K. The diffraction intensity of ZnFe2O4 is an exact complement to the inelastic scattering intensity of several chromate spinel systems which are regarded as model classical spin liquids. Our results challenge this attribution, and suggest instead of the six-spin ring mode, spin excitations in chromate spinels are closely related to the (1, 0, $\frac{1}{2}$) type of spin order and the four-spin ferromagnetic cluster locally at one tetrahedron.},
doi = {10.1103/physrevb.109.064421},
journal = {Physical Review. B},
number = 6,
volume = 109,
place = {United States},
year = {Fri Feb 23 00:00:00 EST 2024},
month = {Fri Feb 23 00:00:00 EST 2024}
}

Works referenced in this record:

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


Direct Visualization of Magnetic Correlations in Frustrated Spinel ZnFe2O4
journal, December 2022

  • Sandemann, Jonas Ruby; Grønbech, Thomas Bjørn Egede; Støckler, Kristoffer Andreas Holm
  • Advanced Materials, Vol. 35, Issue 5
  • DOI: 10.1002/adma.202207152

Tetrahedral Magnetic Order and the Metal-Insulator Transition in the Pyrochlore Lattice of Cd 2 Os 2 O 7
journal, June 2012


Integration of neutron time-of-flight single-crystal Bragg peaks in reciprocal space
journal, May 2014

  • Schultz, Arthur J.; Jørgensen, Mads Ry Vogel; Wang, Xiaoping
  • Journal of Applied Crystallography, Vol. 47, Issue 3
  • DOI: 10.1107/S1600576714006372

The partially disordered state of the frustrated face-centred cubic antiferromagnet
journal, January 1999


Implementation of cross correlation for energy discrimination on the time-of-flight spectrometer CORELLI
journal, March 2018


Magnetism of crystalline and nanostructured ZnFe2O4
journal, August 2000


Spin liquid state in ZnFe2O4
journal, September 1999


Approaching the quantum critical point in a highly correlated all-in–all-out antiferromagnet
journal, June 2020


Models of the magnetic structure of zinc ferrite
journal, May 1970


Neutron Diffraction Studies of Zinc Ferrite and Nickel Ferrite
journal, January 1953


Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr 2 O 4
journal, April 2018


Emergent excitations in a geometrically frustrated magnet
journal, August 2002


Magnetic frustration in a metallic fcc lattice
journal, February 2020


Antiferromagnetism of Zn0.87Mn0.13Fe2O4
journal, January 1970


Crystal structures of spin-Jahn–Teller-ordered MgCr 2 O 4 and ZnCr 2 O 4
journal, July 2013

  • Kemei, Moureen C.; Barton, Phillip T.; Moffitt, Stephanie L.
  • Journal of Physics: Condensed Matter, Vol. 25, Issue 32
  • DOI: 10.1088/0953-8984/25/32/326001

Magnetic neutron scattering measurements on a single crystal of frustrated ZnFe 2 O 4
journal, July 2003


Jana2020 – a new version of the crystallographic computing system Jana
journal, April 2023

  • Petříček, Václav; Palatinus, Lukáš; Plášil, Jakub
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 238, Issue 7-8
  • DOI: 10.1515/zkri-2023-0005

CrystalPlan : an experiment-planning tool for crystallography
journal, March 2011

  • Zikovsky, Janik; Peterson, Peter F.; Wang, Xiaoping P.
  • Journal of Applied Crystallography, Vol. 44, Issue 2
  • DOI: 10.1107/S0021889811007102

Properties of a Classical Spin Liquid: The Heisenberg Pyrochlore Antiferromagnet
journal, March 1998


Controlling inversion disorder in a stoichiometric spinel magnet
journal, October 2022

  • Dronova, Margarita G.; Ye, Feng; Cooper, Scott E.
  • Proceedings of the National Academy of Sciences, Vol. 119, Issue 43
  • DOI: 10.1073/pnas.2208748119

Incommensurate antiferromagnetism in a pure spin system via cooperative organization of local and itinerant moments
journal, February 2013

  • Feng, Yejun; Wang, Jiyang; Silevitch, D. M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 9
  • DOI: 10.1073/pnas.1217292110

Ordering and Antiferromagnetism in Ferrites
journal, May 1956


Magnetic properties of the Zn Fe 2 O 4 spinel
journal, April 1996


A continuous metal-insulator transition driven by spin correlations
journal, May 2021


Local Spin Resonance and Spin-Peierls-like Phase Transition in a Geometrically Frustrated Antiferromagnet
journal, April 2000


Neutron scattering study of the charge-density wave transitions in 2 H Ta Se 2 and 2 H Nb Se 2
journal, July 1977


Magnetic pyrochlore oxides
journal, January 2010

  • Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E.
  • Reviews of Modern Physics, Vol. 82, Issue 1
  • DOI: 10.1103/RevModPhys.82.53

Spin-Lattice Order in Frustrated ZnCr 2 O 4
journal, July 2009


Structure magnétique du spinelle antiferromagneétique ZnFe2O4
journal, January 1970


Accuracy of single-crystal time-of-flight neutron diffraction: a comparative study of MnF2
journal, December 1988

  • Jauch, W.; Schultz, A. J.; Schneider, J. R.
  • Journal of Applied Crystallography, Vol. 21, Issue 6
  • DOI: 10.1107/S0021889888009318

Use of Extinction Corrections in Neutron Diffraction Experiments
journal, January 1988

  • Delapalme, A.
  • Australian Journal of Physics, Vol. 41, Issue 3
  • DOI: 10.1071/PH880383

Bilbao Crystallographic Server: I. Databases and crystallographic computing programs
journal, January 2006

  • Aroyo, Mois Ilia; Perez-Mato, Juan Manuel; Capillas, Cesar
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 221, Issue 1
  • DOI: 10.1524/zkri.2006.221.1.15

Representation analysis of magnetic structures
journal, January 1968

  • Bertaut, E. F.
  • Acta Crystallographica Section A: Crystal Physics, Diffraction, Theoretical and General Crystallography, Vol. 24, Issue 1
  • DOI: 10.1107/S0567739468000306

Improving the accuracy and resolution of neutron crystallographic data by three-dimensional profile fitting of Bragg peaks in reciprocal space
journal, October 2018

  • Sullivan, Brendan; Archibald, Rick; Langan, Patricia S.
  • Acta Crystallographica Section D Structural Biology, Vol. 74, Issue 11
  • DOI: 10.1107/S2059798318013347

Neutron scattering sum rules, symmetric exchanges, and helicoidal magnetism in MnSb2O6
journal, April 2023


A neutron diffraction study of the structure of L-glutamic acid.HCl
journal, August 1972

  • Sequeira, A.; Rajagopal, H.; Chidambaram, R.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 8
  • DOI: 10.1107/S0567740872006399

Magnetic space and superspace groups, representation analysis: competing or friendly concepts?
journal, September 2010

  • Petříček, Václav; Fuksa, Jiří; Dušek, Michal
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 66, Issue 6
  • DOI: 10.1107/S0108767310030527

Magnetic Properties of ZnFe2O4as a 3-D Geometrical Spin Frustration System
journal, October 2004

  • Usa, Toshihiro; Kamazawa, Kazuya; Sekiya, Hirofumi
  • Journal of the Physical Society of Japan, Vol. 73, Issue 10
  • DOI: 10.1143/JPSJ.73.2834

Emergence of Highly Degenerate Excited States in the Frustrated Magnet MgCr 2 O 4
journal, February 2013


Antisymmetric linear magnetoresistance and the planar Hall effect
journal, January 2020


Phase transitions, partial disorder and multi- k structures in Gd 2 Ti 2 O 7
journal, July 2004


High-resolution neutron crystallographic studies of the hydration of the coenzyme cob(II)alamin
journal, May 2011

  • Jogl, Gerwald; Wang, Xiaoping; Mason, Sax A.
  • Acta Crystallographica Section D Biological Crystallography, Vol. 67, Issue 6
  • DOI: 10.1107/S090744491101496X

Large extinction effects in magnesium oxide
journal, March 1973


Magnetic Excitations of the Classical Spin Liquid MgCr 2 O 4
journal, March 2019


Multispin Axis Structures for Antiferromagnets
journal, August 1958


An Antiferromagnetic Transition in Zinc Ferrite
journal, June 1956


Benchmark Crystal Structure of Defect-Free Spinel ZnFe2O4
journal, September 2023

  • Sandemann, Jonas Ruby; Støckler, Kristoffer Andreas Holm; Wang, Xiaoping
  • Journal of the American Chemical Society, Vol. 145, Issue 38
  • DOI: 10.1021/jacs.3c07334

Extinction correction in white X-ray and neutron diffraction
journal, July 1980

  • Tomiyoshi, S.; Yamada, M.; Watanabe, H.
  • Acta Crystallographica Section A: Crystal Physics, Diffraction, Theoretical and General Crystallography, Vol. 36, Issue 4
  • DOI: 10.1107/S0567739480001283

Electronic Conduction of Magnetite (Fe3O4) and its Transition Point at Low Temperatures
journal, August 1939