Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8

Pokharel, G.; May, A. F.; Parker, D. S.; Calder, S.; Ehlers, G.; Huq, A.; Kimber, S. A.  J.; Arachchige, H. Suriya; Poudel, L.; McGuire, M. A.; Mandrus, D.; Christianson, A. D.

doi:10.1103/PhysRevB.97.134117

Title: Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material ${LiGaCr}_{4} S_{8}$

Abstract

In this paper, the physical properties of the spinel LiGaCr₄S₈ have been studied with neutron diffraction, x-ray diffraction, magnetic susceptibility, and heat capacity measurements. The neutron diffraction and synchrotron x-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First-principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. Finally, these results indicate strong magnetoelastic coupling in LiGaCr₄S₈.

Authors:

Pokharel, G. ^[1]; May, A. F. ^[2]; Parker, D. S. ^[2]; Calder, S. ^[3]; Ehlers, G. ^[4]; Huq, A. ^[3]; Kimber, S. A. J. ^[3]; Arachchige, H. Suriya ^[1]; Poudel, L. ^[5]; McGuire, M. A. ^[2]; Mandrus, D. ^[6]; Christianson, A. D. ^[7]

Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Technologies Division
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division; Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering; National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy. Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division. Neutron Scattering Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy

Publication Date:: Mon Apr 30 00:00:00 EDT 2018

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Gordon and Betty Moore Foundation (United States)

OSTI Identifier:: 1435213

Alternate Identifier(s):: OSTI ID: 1435378

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357; GBMF4416

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 97; Journal Issue: 13; 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; frustrated magnetism; magnetic susceptibility; magnetism; structural properties

Citation Formats


                    Pokharel, G., May, A. F., Parker, D. S., Calder, S., Ehlers, G., Huq, A., Kimber, S. A.  J., Arachchige, H. Suriya, Poudel, L., McGuire, M. A., Mandrus, D., and Christianson, A. D. Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8.  United States: N. p., 2018. 
Web.  doi:10.1103/PhysRevB.97.134117.

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                    Pokharel, G., May, A. F., Parker, D. S., Calder, S., Ehlers, G., Huq, A., Kimber, S. A.  J., Arachchige, H. Suriya, Poudel, L., McGuire, M. A., Mandrus, D., & Christianson, A. D. Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8.  United States.  https://doi.org/10.1103/PhysRevB.97.134117

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                    Pokharel, G., May, A. F., Parker, D. S., Calder, S., Ehlers, G., Huq, A., Kimber, S. A.  J., Arachchige, H. Suriya, Poudel, L., McGuire, M. A., Mandrus, D., and Christianson, A. D. Mon .  
"Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8".  United States.  https://doi.org/10.1103/PhysRevB.97.134117.  https://www.osti.gov/servlets/purl/1435213.

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@article{osti_1435213,

  title        = {Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8},

  author       = {Pokharel, G. and May, A. F. and Parker, D. S. and Calder, S. and Ehlers, G. and Huq, A. and Kimber, S. A.  J. and Arachchige, H. Suriya and Poudel, L. and McGuire, M. A. and Mandrus, D. and Christianson, A. D.},

  abstractNote = {In this paper, the physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, x-ray diffraction, magnetic susceptibility, and heat capacity measurements. The neutron diffraction and synchrotron x-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First-principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. Finally, these results indicate strong magnetoelastic coupling in LiGaCr4S8.},

  doi          = {10.1103/PhysRevB.97.134117},

  journal      = {Physical Review B},

  number       = 13,

  volume       = 97,

  place        = {United States},

  year         = {Mon Apr 30 00:00:00 EDT 2018},

  month        = {Mon Apr 30 00:00:00 EDT 2018}

}

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https://doi.org/10.1103/PhysRevB.97.134117

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Cited by: 35 works

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Figures / Tables:

FIG. 1.: Crystal structure of LiGaCr₄S₈ depicting the breathing pyrochlore Cr sublattice. The exchange interactions within the small and large tetrahedra are labeled J₁ and J′₁ respectively. J₂ denotes the next nearest neighbor exchange interaction.

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Works referenced in this record:

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Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg Hamiltonians
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Spin ordering induced by lattice distortions in classical Heisenberg antiferromagnets on the breathing pyrochlore lattice
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Title: Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr 4 S 8

Abstract

Citation Formats

Figures / Tables:

Orbital physics in sulfur spinels: ordered, liquid and glassy ground states journal, January 2004

Thermal study of the interplay between spin and lattice in CoCr 2 O 4 and CdCr 2 O 4 journal, February 2013

Generalized Gradient Approximation Made Simple journal, October 1996

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Statics and Dynamics of Incommensurate Spin Order in a Geometrically Frustrated Antiferromagnet CdCr 2 O 4 journal, December 2005

EXPGUI , a graphical user interface for GSAS journal, April 2001

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Spin-Driven Phonon Splitting in Bond-Frustrated ZnCr 2 S 4 journal, August 2006

Spin and Orbital Frustration in MnSc 2 S 4 and FeSc 2 S 4 journal, March 2004

Some new mixed A-site chromium chalcogenide spinels journal, June 1970

Probing Spin Correlations with Phonons in the Strongly Frustrated Magnet ZnCr 2 O 4 journal, April 2005

FeCr2S4 in magnetic fields: possible evidence for a multiferroic ground state journal, August 2014

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Gitterschwingungsspektren XVIII. Chromthio- und Chromselenospinelle mit 1:1-Ordnung auf den Tetraederplätzen journal, October 1977

Experimental realization of a quantum breathing pyrochlore antiferromagnet journal, August 2014

Negative thermal expansion and magnetostriction in the frustrated spinel ZnCr 2 (Se 1− x S x ) 4 (0 ≤ x ≤ 0.1) journal, April 2016

Spin-glass-like behavior in single-crystalline Cu 0.44 In 0.48 Cr 1.95 Se 4 journal, January 2008

Electronic band structure and exchange coupling constants in A Cr 2 X 4 spinels ( A = Zn , Cd, Hg; X = O , S, Se) journal, March 2008

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Large Magnetostriction and Negative Thermal Expansion in the Frustrated Antiferromagnet ZnCr 2 Se 4 journal, April 2007

FeCr$_2$S$_4$ in magnetic fields: possible evidence for a multiferroic ground state text, January 2013

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Title: Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material ${LiGaCr}_{4} S_{8}$

Orbital physics in sulfur spinels: ordered, liquid and glassy ground states
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journal, February 2013

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Breathing Pyrochlore Lattice Realized in $A$ -Site Ordered Spinel Oxides ${LiGaCr}_{4} O_{8}$ and ${LiInCr}_{4} O_{8}$
journal, February 2013

Magnetic and Structural Properties of A-Site Ordered Chromium Spinel Sulfides: Alternating Antiferromagnetic and Ferromagnetic Interactions in the Breathing Pyrochlore Lattice
journal, March 2018

Magnetodielectric effects in $A$ -site cation-ordered chromate spinels $Li M C r_{4} O_{8}$ ( $M = Ga$ and In)
journal, August 2016

Néel-type skyrmion lattice with confined orientation in the polar magnetic semiconductor GaV4S8
journal, September 2015

Spin-lattice coupling in the frustrated antiferromagnet ZnCr $_{2}$ Se $_{4}$ probed by ultrasound
journal, September 2012

Statics and Dynamics of Incommensurate Spin Order in a Geometrically Frustrated Antiferromagnet ${CdCr}_{2} O_{4}$
journal, December 2005

EXPGUI , a graphical user interface for GSAS
journal, April 2001

Weyl magnons in breathing pyrochlore antiferromagnets
journal, September 2016

Colossal Magnetocapacitance and Colossal Magnetoresistance in ${HgCr}_{2} S_{4}$
journal, April 2006

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Orbital Freezing and Orbital Glass State in $F e {C r}_{2} S_{4}$
journal, January 2005

Ferromagnetism versus Antiferromagnetism in Face-Centered-Cubic Iron
journal, May 1986

Complex magnetostructural order in the frustrated spinel ${LiInCr}_{4} O_{8}$
journal, May 2015

Anisotropic Exchange within Decoupled Tetrahedra in the Quantum Breathing Pyrochlore ${Ba}_{3} {Yb}_{2} {Zn}_{5} O_{11}$
journal, June 2016

Multistage symmetry breaking in the breathing pyrochlore lattice ${Li (Ga, In) Cr}_{4} O_{8}$
journal, May 2016

Exchange Interactions in Ferromagnetic Chromium Chalcogenide Spinels
journal, November 1966

Low-energy excitations and ground-state selection in the quantum breathing pyrochlore antiferromagnet ${Ba}_{3} {Yb}_{2} {Zn}_{5} O_{11}$
journal, June 2016

Spin-Driven Phonon Splitting in Bond-Frustrated ${ZnCr}_{2} S_{4}$
journal, August 2006

Spin and Orbital Frustration in ${MnSc}_{2} S_{4}$ and ${FeSc}_{2} S_{4}$
journal, March 2004

Some new mixed A-site chromium chalcogenide spinels
journal, June 1970

Probing Spin Correlations with Phonons in the Strongly Frustrated Magnet ${ZnCr}_{2} O_{4}$
journal, April 2005

FeCr2S4 in magnetic fields: possible evidence for a multiferroic ground state
journal, August 2014

Quantum spin ice on the breathing pyrochlore lattice
journal, August 2016

Gitterschwingungsspektren XVIII. Chromthio- und Chromselenospinelle mit 1:1-Ordnung auf den Tetraederplätzen
journal, October 1977

Experimental realization of a quantum breathing pyrochlore antiferromagnet
journal, August 2014

Negative thermal expansion and magnetostriction in the frustrated spinel ZnCr ₂ (Se _{1− x} S _x ) ₄ (0 ≤ x ≤ 0.1)
journal, April 2016

Spin-glass-like behavior in single-crystalline ${Cu}_{0.44} {In}_{0.48} {Cr}_{1.95} {Se}_{4}$
journal, January 2008

Electronic band structure and exchange coupling constants in $A {Cr}_{2} X_{4}$ spinels ( $A = Zn$ , Cd, Hg; $X = O$ , S, Se)
journal, March 2008

Magnetic phase diagram of the helimagnetic spinel compound ZnCr ₂ Se ₄ revisited by small-angle neutron scattering
journal, March 2016

Large Magnetostriction and Negative Thermal Expansion in the Frustrated Antiferromagnet ${ZnCr}_{2} {Se}_{4}$
journal, April 2007

FeCr$_2$S$_4$ in magnetic fields: possible evidence for a multiferroic ground state
text, January 2013

Quantum spin ice on the breathing pyrochlore lattice
text, January 2015

Magnetic phase diagram of the helimagnetic spinel compound ZnCr2Se4 revisited by small-angle neutron scattering
text, January 2016

Magnetic and Structural Properties of A-Site Ordered Chromium Spinel Sulfides: Alternating Antiferromagnetic and Ferromagnetic Interactions in the Breathing Pyrochlore Lattice
text, January 2018

Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg Hamiltonians
journal, December 2019

Formation of breathing pyrochlore lattices: structural, thermodynamic and crystal chemical aspects
journal, January 2020

Spin ordering induced by lattice distortions in classical Heisenberg antiferromagnets on the breathing pyrochlore lattice
journal, April 2019

Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg Hamiltonians
text, January 2019

Behavior of the breathing pyrochlore lattice Ba$_3$Yb$_2$Zn$_5$O$_{11}$ in applied magnetic field
text, January 2018