Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7

J. Gaudet; E. M. Smith; J. Dudemaine; J. Beare; C. R.C. Buhariwalla; N. P. Butch; M. B. Stone; A. I. Kolesnikov; Guangyong Xu; D. R. Yahne; K. A. Ross; C. A. Marjerrison; J. D. Garrett; G. M. Luke; A. D. Bianchi; B. D. Gaulin

doi:10.1103/PhysRevLett.122.187201

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7

J. Gaudet, E. M. Smith, J. Dudemaine, J. Beare, C. R.C. Buhariwalla, N. P. Butch, M. B. Stone, A. I. Kolesnikov, Guangyong Xu, D. R. Yahne, K. A. Ross, C. A. Marjerrison, J. D. Garrett, G. M. Luke, A. D. Bianchi, B. D. Gaulin

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Abstract

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. 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 lowerature behavior of this material.

Original language	English
Article number	187201
Journal	Physical Review Letters
Volume	122
Issue number	18
DOIs	https://doi.org/10.1103/PhysRevLett.122.187201
State	Published - May 7 2019

Funding

We acknowledge useful conversations with Allen Scheie, Alannah Hallas, and Owen Benton. We greatly appreciate the technical support from Alan Ye and Yegor Vekhov at the NIST Center for Neutron Research. This work was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). A portion of this research used resources at the High Flux Isotope Reactor and Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. We also acknowledge the support of the National Institute of Standards and Technology, U.S. Department of Commerce. Certain commercial equipment, instruments, or materials (or suppliers, or software, etc.) are identified in this Letter to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose.

Funders	Funder number
National Institute of Standards and Technology
Natural Sciences and Engineering Research Council of Canada
U.S. Department of Commerce

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10.1103/PhysRevLett.122.187201

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Gaudet, J., Smith, E. M., Dudemaine, J., Beare, J., Buhariwalla, C. R. C., Butch, N. P., Stone, M. B., Kolesnikov, A. I., Xu, G., Yahne, D. R., Ross, K. A., Marjerrison, C. A., Garrett, J. D., Luke, G. M., Bianchi, A. D., & Gaulin, B. D. (2019). Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7. Physical Review Letters, 122(18), Article 187201. https://doi.org/10.1103/PhysRevLett.122.187201

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title = "Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7",

abstract = "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. 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 lowerature behavior of this material.",

author = "J. Gaudet and Smith, {E. M.} and J. Dudemaine and J. Beare and Buhariwalla, {C. R.C.} and Butch, {N. P.} and Stone, {M. B.} and Kolesnikov, {A. I.} and Guangyong Xu 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.}",

note = "Publisher Copyright: {\textcopyright} 2019 American Physical Society.",

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doi = "10.1103/PhysRevLett.122.187201",

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Gaudet, J, Smith, EM, Dudemaine, J, Beare, J, Buhariwalla, CRC, Butch, NP, Stone, MB , Kolesnikov, AI, Xu, G, Yahne, DR, Ross, KA, Marjerrison, CA, Garrett, JD, Luke, GM, Bianchi, AD & Gaulin, BD 2019, 'Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7', Physical Review Letters, vol. 122, no. 18, 187201. https://doi.org/10.1103/PhysRevLett.122.187201

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T1 - Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7

AU - Gaudet, J.

AU - Smith, E. M.

AU - Dudemaine, J.

AU - Beare, J.

AU - Buhariwalla, C. R.C.

AU - Butch, N. P.

AU - Stone, M. B.

AU - Kolesnikov, A. I.

AU - Xu, Guangyong

AU - Yahne, D. R.

AU - Ross, K. A.

AU - Marjerrison, C. A.

AU - Garrett, J. D.

AU - Luke, G. M.

AU - Bianchi, A. D.

AU - Gaulin, B. D.

PY - 2019/5/7

Y1 - 2019/5/7

N2 - 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. 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 lowerature behavior of this material.

AB - 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. 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 lowerature behavior of this material.

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Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce2Zr2 O7

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