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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 LiGaCr 4S 8 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 LiGaCr 4S 8.

Authors:
 [1];  [2];  [2];  [3];  [4];  [3];  [3];  [1];  [5];  [2];  [6];  [7]
  1. 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
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Technologies Division
  5. 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
  6. 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
  7. 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:
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) (SC-22); 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.
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. doi:10.1103/PhysRevB.97.134117.
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. doi:10.1103/PhysRevB.97.134117. https://www.osti.gov/servlets/purl/1435213.
@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 = {2018},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 5 works
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Figures / Tables:

FIG. 1. 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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