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Title: Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2O7

Abstract

Neutron scattering measurements on the pyrochlore magnet Ce 2 Zr 2 O 7 reveal an unusual crystal field splitting of its lowest J = 5 / 2 multiplet, such that its ground-state doublet is composed of m J = ± 3 / 2 , giving these doublets a dipole-octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θ CW = - 0.4 ( 2 ) K , leading to a naive expectation of an all-in, all-out ordered state at low temperatures. Instead, our low-energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q|=0 , and no long-range order at low temperatures. We find that this is consistent with recent theory predicting symmetry-enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce 2 Zr 2 O 7 and could play an important role in the low-temperature behavior of this material.

Authors:
 [1];  [1];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4];  [3];  [5];  [6];  [7];  [7];  [8];  [9];  [10]
  1. McMaster Univ., Hamilton, ON (Canada)
  2. Univ. de Montreal, QC (Canada)
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Colorado State Univ., Fort Collins, CO (United States)
  6. Colorado State Univ., Fort Collins, CO (United States); Canadian Inst. for Advanced Research, Toronto, ON (Canada)
  7. McMaster Univ., Hamilton, ON (Canada). Brockhouse Inst. for Materials Research
  8. McMaster Univ., Hamilton, ON (Canada); Canadian Inst. for Advanced Research, Toronto, ON (Canada)
  9. Univ. de Montreal, QC (Canada); Regroupement Quebecois sur les Materiaux de Pointe (RQMP), Quebec, QC (Canada)
  10. McMaster Univ., Hamilton, ON (Canada); Canadian Inst. for Advanced Research, Toronto, ON (Canada); McMaster Univ., Hamilton, ON (Canada). Brockhouse Inst. for Materials Research
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); Natural Sciences and Engineering Research Council of Canada (NSERC)
OSTI Identifier:
1666021
Alternate Identifier(s):
OSTI ID: 1511095
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 122; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Frustrated magnetism; quantum spin liquid; spin dynamics; pyrochlore; neutron scattering

Citation Formats

Gaudet, J., Smith, E.  M., Dudemaine, J., Beare, J., Buhariwalla, C.  R. C., Butch, N.  P., Stone, M.  B., Kolesnikov, A.  I., Xu, Guangyong, Yahne, D.  R., Ross, K.  A., Marjerrison, C.  A., Garrett, J.  D., Luke, G.  M., Bianchi, A.  D., and Gaulin, B.  D. Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2O7. United States: N. p., 2019. Web. doi:10.1103/physrevlett.122.187201.
Gaudet, J., Smith, E.  M., Dudemaine, J., Beare, J., Buhariwalla, C.  R. C., Butch, N.  P., Stone, M.  B., Kolesnikov, A.  I., Xu, Guangyong, Yahne, D.  R., Ross, K.  A., Marjerrison, C.  A., Garrett, J.  D., Luke, G.  M., Bianchi, A.  D., & Gaulin, B.  D. Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2O7. United States. https://doi.org/10.1103/physrevlett.122.187201
Gaudet, J., Smith, E.  M., Dudemaine, J., Beare, J., Buhariwalla, C.  R. C., Butch, N.  P., Stone, M.  B., Kolesnikov, A.  I., Xu, Guangyong, Yahne, D.  R., Ross, K.  A., Marjerrison, C.  A., Garrett, J.  D., Luke, G.  M., Bianchi, A.  D., and Gaulin, B.  D. Tue . "Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2O7". United States. https://doi.org/10.1103/physrevlett.122.187201. https://www.osti.gov/servlets/purl/1666021.
@article{osti_1666021,
title = {Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2O7},
author = {Gaudet, J. and Smith, E.  M. and Dudemaine, J. and Beare, J. and Buhariwalla, C.  R. C. and Butch, N.  P. and Stone, M.  B. and Kolesnikov, A.  I. and Xu, Guangyong and Yahne, D.  R. and Ross, K.  A. and Marjerrison, C.  A. and Garrett, J.  D. and Luke, G.  M. and Bianchi, A.  D. and Gaulin, B.  D.},
abstractNote = {Neutron scattering measurements on the pyrochlore magnet Ce2Zr2O7 reveal an unusual crystal field splitting of its lowest J=5/2 multiplet, such that its ground-state doublet is composed of mJ=±3/2, giving these doublets a dipole-octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θCW=-0.4(2) K, leading to a naive expectation of an all-in, all-out ordered state at low temperatures. Instead, our low-energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q|=0, and no long-range order at low temperatures. We find that this is consistent with recent theory predicting symmetry-enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce2Zr2O7 and could play an important role in the low-temperature behavior of this material.},
doi = {10.1103/physrevlett.122.187201},
journal = {Physical Review Letters},
number = 18,
volume = 122,
place = {United States},
year = {Tue May 07 00:00:00 EDT 2019},
month = {Tue May 07 00:00:00 EDT 2019}
}

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