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Title: Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore

Abstract

A quantum spin liquid is a state of matter where unpaired electrons’ spins, although entangled, do not show magnetic order even at the zero temperature. The realization of a quantum spin liquid is a long-sought goal in condensed-matter physics. Although neutron scattering experiments on the two-dimensional spin-1/2 kagome lattice ZnCu3(OD)6Cl2 and triangular lattice YbMgGaO4 have found evidence for the hallmark of a quantum spin liquid at very low temperature (a continuum of magnetic excitations), the presence of magnetic and non-magnetic site chemical disorder complicates the interpretation of the data. Recently, the three-dimensional Ce3+ pyrochlore lattice Ce2Sn2O7 has been suggested as a clean, effective spin-1/2 quantum spin liquid candidate, but evidence of a spin excitation continuum is still missing. Furthermore, we use thermodynamic, muon spin relaxation and neutron scattering experiments on single crystals of Ce2Zr2O7, a compound isostructural to Ce2Sn2O7, to demonstrate the absence of magnetic ordering and the presence of a spin excitation continuum at 35 mK. With no evidence of oxygen deficiency and magnetic/non-magnetic ion disorder seen by neutron diffraction and diffuse scattering measurements, Ce2Zr2O7 may be a three-dimensional pyrochlore lattice quantum spin liquid material with minimum magnetic and non-magnetic chemical disorder.

Authors:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4];  [5];  [5];  [1];  [1];  [6];  [6];  [7];  [7];  [2];  [1] more »;  [1]; ORCiD logo [8]; ORCiD logo [1] « less
  1. Rice Univ., Houston, TX (United States)
  2. Univ. of California, San Diego, CA (United States)
  3. STFC Rutherford-Appleton Lab, Didcot (United Kingdom)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  6. Rutgers Univ., Piscataway, NJ (United States)
  7. Quantum Design Inc., San Diego, CA (United States)
  8. The Univ. of Hong Kong, Hong Kong (China); Fudan Univ., Shanghai (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1558477
Alternate Identifier(s):
OSTI ID: 1661263
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 15; Journal Issue: 7; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Gao, Bin, Chen, Tong, Tam, David W., Huang, Chien -Lung, Sasmal, Kalyan, Adroja, Devashibhai T., Ye, Feng, Cao, Huibo, Sala, Gabriele, Stone, Matthew B., Baines, Christopher, Verezhak, Joel A. T., Hu, Haoyu, Chung, Jae -Ho, Xu, Xianghan, Cheong, Sang -Wook, Nallaiyan, Manivannan, Spagna, Stefano, Maple, M. Brian, Nevidomskyy, Andriy H., Morosan, Emilia, Chen, Gang, and Dai, Pengcheng. Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore. United States: N. p., 2019. Web. doi:10.1038/s41567-019-0577-6.
Gao, Bin, Chen, Tong, Tam, David W., Huang, Chien -Lung, Sasmal, Kalyan, Adroja, Devashibhai T., Ye, Feng, Cao, Huibo, Sala, Gabriele, Stone, Matthew B., Baines, Christopher, Verezhak, Joel A. T., Hu, Haoyu, Chung, Jae -Ho, Xu, Xianghan, Cheong, Sang -Wook, Nallaiyan, Manivannan, Spagna, Stefano, Maple, M. Brian, Nevidomskyy, Andriy H., Morosan, Emilia, Chen, Gang, & Dai, Pengcheng. Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore. United States. https://doi.org/10.1038/s41567-019-0577-6
Gao, Bin, Chen, Tong, Tam, David W., Huang, Chien -Lung, Sasmal, Kalyan, Adroja, Devashibhai T., Ye, Feng, Cao, Huibo, Sala, Gabriele, Stone, Matthew B., Baines, Christopher, Verezhak, Joel A. T., Hu, Haoyu, Chung, Jae -Ho, Xu, Xianghan, Cheong, Sang -Wook, Nallaiyan, Manivannan, Spagna, Stefano, Maple, M. Brian, Nevidomskyy, Andriy H., Morosan, Emilia, Chen, Gang, and Dai, Pengcheng. Mon . "Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore". United States. https://doi.org/10.1038/s41567-019-0577-6. https://www.osti.gov/servlets/purl/1558477.
@article{osti_1558477,
title = {Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore},
author = {Gao, Bin and Chen, Tong and Tam, David W. and Huang, Chien -Lung and Sasmal, Kalyan and Adroja, Devashibhai T. and Ye, Feng and Cao, Huibo and Sala, Gabriele and Stone, Matthew B. and Baines, Christopher and Verezhak, Joel A. T. and Hu, Haoyu and Chung, Jae -Ho and Xu, Xianghan and Cheong, Sang -Wook and Nallaiyan, Manivannan and Spagna, Stefano and Maple, M. Brian and Nevidomskyy, Andriy H. and Morosan, Emilia and Chen, Gang and Dai, Pengcheng},
abstractNote = {A quantum spin liquid is a state of matter where unpaired electrons’ spins, although entangled, do not show magnetic order even at the zero temperature. The realization of a quantum spin liquid is a long-sought goal in condensed-matter physics. Although neutron scattering experiments on the two-dimensional spin-1/2 kagome lattice ZnCu3(OD)6Cl2 and triangular lattice YbMgGaO4 have found evidence for the hallmark of a quantum spin liquid at very low temperature (a continuum of magnetic excitations), the presence of magnetic and non-magnetic site chemical disorder complicates the interpretation of the data. Recently, the three-dimensional Ce3+ pyrochlore lattice Ce2Sn2O7 has been suggested as a clean, effective spin-1/2 quantum spin liquid candidate, but evidence of a spin excitation continuum is still missing. Furthermore, we use thermodynamic, muon spin relaxation and neutron scattering experiments on single crystals of Ce2Zr2O7, a compound isostructural to Ce2Sn2O7, to demonstrate the absence of magnetic ordering and the presence of a spin excitation continuum at 35 mK. With no evidence of oxygen deficiency and magnetic/non-magnetic ion disorder seen by neutron diffraction and diffuse scattering measurements, Ce2Zr2O7 may be a three-dimensional pyrochlore lattice quantum spin liquid material with minimum magnetic and non-magnetic chemical disorder.},
doi = {10.1038/s41567-019-0577-6},
journal = {Nature Physics},
number = 7,
volume = 15,
place = {United States},
year = {2019},
month = {7}
}

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Cited by: 11 works
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Figures / Tables:

Figure 1 Figure 1: Summary of crystal structure, CEF levels, direct-current (dc) susceptibility, and specific heat of Ce2Zr2O7. a, Schematic structure of Ce2Zr2O7 with lattice parameters a = b = c = 10.71 Å. The blue ions are magnetic Ce3+ (A site) and the red ions are nonmagnetic Zr4+ (B site). b,more » Inelastic neutron scattering from powder samples of Ce2Zr2O7 with incident neutron beam energy of Ei= 250 meV at 5 K. Phonons and other background scattering measured in nonmagnetic analog La2Zr2O7 were subtracted. Two Kramer’s doublets at 55.8 and 110.8 meV are clearly seen. c, The dc magnetic susceptibility χ (blue) and 1/χ (red). The applied field is 1 kOe along the [1,1,1] direction. The black dashed lines are low-high temperature Curie-Weiss fit to the data. The red curve in the inset shows energy dependence of the CEF levels for integrated wave vectors from 4 to 6 Å-1. The solid black lines in inset and main panel are CEF fits to the data. d, Magnetization (M) as a function of applied magnetic field (H) in Tesla along the [1,1,1] direction at different temperatures. e, Magnetic contribution to specific heat Cmag for different magnetic fields along the [1,1,1] direction. The lattice contribution Cphonon has been subtracted. f, Cmag/T versus T plot and the magnetic entropy Smag calculated from Cmag/T in zero field. Smag reaches the entropy for a two level system (Rln2) instead of the spin ice entropy (1-(1/2)(ln(3/2)/ln2) Rln2. The inset shows C/T versus T2 plot. Data between 10 and 20 K are fit with Cphonon/T = β T2 + αT4.« less

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