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Title: Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8

Abstract

We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high- and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parametrize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualitative agreement with density-functional-theory predictions [Ghosh et al., npj Quantum Mater. 4, 63 (2019)]. We explain the origin of geometrical frustration in LiGaCr4S8 in terms of net antiferromagnetic coupling between emergent tetrahedral spin clusters that occupy a face-centered-cubic lattice. Our results provide insight into the emergence of frustration in the presence of strong further-neighbor couplings, and a blueprint for the determination of magnetic interactions in classical spin liquids.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [2];  [2]; ORCiD logo [2];  [2]; ORCiD logo [2];  [2];  [2];  [3];  [1];  [2];  [2]
+ Show Author Affiliations
  1. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Inst. Laue-Langevin, Grenoble Cedex (France)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1785681
Alternate Identifier(s):
OSTI ID: 1807313
Grant/Contract Number:  
GBMF4416; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 125; Journal Issue: 16; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Exchange interaction; Exotic phases of matter; Magnetic order; Magnetic phase transitions; Magnetic susceptibility; Magnetism; Spin dynamics

Citation Formats

Pokharel, Ganesh, Arachchige, Hasitha Suriya, Williams, Travis J., May, Andrew F., Fishman, Randy S., Sala, Gabriele, Calder, Stuart, Ehlers, Georg, Parker, David S., Hong, Tao, Wildes, Andrew, Mandrus, David, Paddison, Joseph A. M., and Christianson, Andrew D. Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8. United States: N. p., 2020. Web. doi:10.1103/physrevlett.125.167201.
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Pokharel, Ganesh, Arachchige, Hasitha Suriya, Williams, Travis J., May, Andrew F., Fishman, Randy S., Sala, Gabriele, Calder, Stuart, Ehlers, Georg, Parker, David S., Hong, Tao, Wildes, Andrew, Mandrus, David, Paddison, Joseph A. M., & Christianson, Andrew D. Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8. United States. https://doi.org/10.1103/physrevlett.125.167201
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Pokharel, Ganesh, Arachchige, Hasitha Suriya, Williams, Travis J., May, Andrew F., Fishman, Randy S., Sala, Gabriele, Calder, Stuart, Ehlers, Georg, Parker, David S., Hong, Tao, Wildes, Andrew, Mandrus, David, Paddison, Joseph A. M., and Christianson, Andrew D. Fri . "Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8". United States. https://doi.org/10.1103/physrevlett.125.167201. https://www.osti.gov/servlets/purl/1785681.
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@article{osti_1785681,
title = {Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8},
author = {Pokharel, Ganesh and Arachchige, Hasitha Suriya and Williams, Travis J. and May, Andrew F. and Fishman, Randy S. and Sala, Gabriele and Calder, Stuart and Ehlers, Georg and Parker, David S. and Hong, Tao and Wildes, Andrew and Mandrus, David and Paddison, Joseph A. M. and Christianson, Andrew D.},
abstractNote = {We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high- and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parametrize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualitative agreement with density-functional-theory predictions [Ghosh et al., npj Quantum Mater. 4, 63 (2019)]. We explain the origin of geometrical frustration in LiGaCr4S8 in terms of net antiferromagnetic coupling between emergent tetrahedral spin clusters that occupy a face-centered-cubic lattice. Our results provide insight into the emergence of frustration in the presence of strong further-neighbor couplings, and a blueprint for the determination of magnetic interactions in classical spin liquids.},
doi = {10.1103/physrevlett.125.167201},
journal = {Physical Review Letters},
number = 16,
volume = 125,
place = {United States},
year = {Fri Oct 16 00:00:00 EDT 2020},
month = {Fri Oct 16 00:00:00 EDT 2020}
}
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