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Title: Coulomb spin liquid in anion-disordered pyrochlore Tb 2Hf 2O 7

Abstract

Here, the charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. Here we demonstrate in the pyrochlore Tb 2Hf 2O 7, that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5];  [1];  [6]; ORCiD logo [7];  [1];  [1];  [1];  [8];  [8];  [1];  [1]; ORCiD logo [1]; ORCiD logo [3];  [1]; ORCiD logo [1]
  1. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  2. CNRS-Univ. Grenoble Alpes, Grenoble (France)
  3. Univ. of Warwick, Coventry (United Kingdom)
  4. Institut Laue-Langevin, Grenoble (France); STFC Rutherford Appleton Lab., Didcot (United Kingdom)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Univ. Grenoble Alpes, Grenoble (France)
  7. Paul Scherrer Inst. (PSI), Villigen (Switzerland); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  8. STFC Rutherford Appleton Lab., Didcot (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1439954
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sibille, Romain, Lhotel, Elsa, Hatnean, Monica Ciomaga, Nilsen, Goran J., Ehlers, Georg, Cervellino, Antonio, Ressouche, Eric, Frontzek, Matthias D., Zaharko, Oksana, Pomjakushin, Vladimir, Stuhr, Uwe, Walker, Helen C., Adroja, Devashibhai T., Luetkens, Hubertus, Baines, Chris, Amato, Alex, Balakrishnan, Geetha, Fennell, Tom, and Kenzelmann, Michel. Coulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7. United States: N. p., 2017. Web. doi:10.1038/s41467-017-00905-w.
Sibille, Romain, Lhotel, Elsa, Hatnean, Monica Ciomaga, Nilsen, Goran J., Ehlers, Georg, Cervellino, Antonio, Ressouche, Eric, Frontzek, Matthias D., Zaharko, Oksana, Pomjakushin, Vladimir, Stuhr, Uwe, Walker, Helen C., Adroja, Devashibhai T., Luetkens, Hubertus, Baines, Chris, Amato, Alex, Balakrishnan, Geetha, Fennell, Tom, & Kenzelmann, Michel. Coulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7. United States. doi:10.1038/s41467-017-00905-w.
Sibille, Romain, Lhotel, Elsa, Hatnean, Monica Ciomaga, Nilsen, Goran J., Ehlers, Georg, Cervellino, Antonio, Ressouche, Eric, Frontzek, Matthias D., Zaharko, Oksana, Pomjakushin, Vladimir, Stuhr, Uwe, Walker, Helen C., Adroja, Devashibhai T., Luetkens, Hubertus, Baines, Chris, Amato, Alex, Balakrishnan, Geetha, Fennell, Tom, and Kenzelmann, Michel. Thu . "Coulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7". United States. doi:10.1038/s41467-017-00905-w. https://www.osti.gov/servlets/purl/1439954.
@article{osti_1439954,
title = {Coulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7},
author = {Sibille, Romain and Lhotel, Elsa and Hatnean, Monica Ciomaga and Nilsen, Goran J. and Ehlers, Georg and Cervellino, Antonio and Ressouche, Eric and Frontzek, Matthias D. and Zaharko, Oksana and Pomjakushin, Vladimir and Stuhr, Uwe and Walker, Helen C. and Adroja, Devashibhai T. and Luetkens, Hubertus and Baines, Chris and Amato, Alex and Balakrishnan, Geetha and Fennell, Tom and Kenzelmann, Michel},
abstractNote = {Here, the charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. Here we demonstrate in the pyrochlore Tb2Hf2O7, that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.},
doi = {10.1038/s41467-017-00905-w},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {10}
}

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Works referenced in this record:

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  • Payne, Julia L.; Tucker, Matthew G.; Evans, Ivana Radosavljević
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Direct Localization of Atoms in Mixed-Occupancy Powders by Resonant Contrast Diffraction
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Quantum Melting of Spin Ice: Emergent Cooperative Quadrupole and Chirality
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Random Antiferromagnetic Chain
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Anisotropic Propagating Excitations and Quadrupolar Effects in Tb 2 Ti 2 O 7
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Magnetoelastic Excitations in the Pyrochlore Spin Liquid Tb 2 Ti 2 O 7
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Power-Law Spin Correlations in the Pyrochlore Antiferromagnet Tb 2 Ti 2 O 7
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Quasispin Glass in a Geometrically Frustrated Magnet
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    Works referencing / citing this record:

    Direct Localization of Atoms in Mixed-Occupancy Powders by Resonant Contrast Diffraction
    journal, February 2005

    • Palancher, Herve; Hodeau, Jean-Louis; Pichon, Christophe
    • Angewandte Chemie International Edition, Vol. 44, Issue 11
    • DOI: 10.1002/anie.200461642

    Resonating valence bonds: A new kind of insulator?
    journal, February 1973


    Spin-glass-like behavior in Y2Mo2O7, a concentrated, crystalline system with negligible apparent disorder
    journal, September 1986


    Oxide pyrochlores — A review
    journal, January 1983

    • Subramanian, M. A.; Aravamudan, G.; Subba Rao, G. V.
    • Progress in Solid State Chemistry, Vol. 15, Issue 2
    • DOI: 10.1016/0079-6786(83)90001-8

    Transmission electron microscopic study of pyrochlore to defect-fluorite transition in rare-earth pyrohafnates
    journal, October 2012

    • Karthik, Chinnathambi; Anderson, Thomas J.; Gout, Delphine
    • Journal of Solid State Chemistry, Vol. 194
    • DOI: 10.1016/j.jssc.2012.05.008

    From fluorite to pyrochlore: Characterisation of local and average structure of neodymium zirconate, Nd2Zr2O7
    journal, September 2013

    • Payne, Julia L.; Tucker, Matthew G.; Evans, Ivana Radosavljević
    • Journal of Solid State Chemistry, Vol. 205
    • DOI: 10.1016/j.jssc.2013.07.001

    Investigating the Local Structure of Lanthanoid Hafnates Ln 2 Hf 2 O 7 via Diffraction and Spectroscopy
    journal, January 2013

    • Blanchard, Peter E. R.; Liu, Sam; Kennedy, Brendan J.
    • The Journal of Physical Chemistry C, Vol. 117, Issue 5
    • DOI: 10.1021/jp311329q

    Spin liquids in frustrated magnets
    journal, March 2010


    A spin-liquid with pinch-line singularities on the pyrochlore lattice
    journal, May 2016

    • Benton, Owen; Jaubert, L. D. C.; Yan, Han
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms11572

    Quantum magnetism and criticality
    journal, March 2008


    Nonlinear susceptibility measurements at the spin-glass transition of the pyrochlore antiferromagnet Y2Mo2O7
    journal, January 1996

    • Gingras, M. J. P.; Stager, C. V.; Gaulin, B. D.
    • Journal of Applied Physics, Vol. 79, Issue 8
    • DOI: 10.1063/1.362062

    Spin freezing in the pyrochlore antiferromagnet Pr 2 Zr 2 O 7
    journal, January 2009


    Absence of spin-ice state in the disordered fluorite D y 2 Z r 2 O 7
    journal, June 2019


    Disorder in Pyrochlore Oxides
    journal, August 2000


    Oxide Ion Disorder in Nd2Hf2O7: Oxide Ion Disorder in Nd2Hf2O7
    journal, December 2007


    Spin Ice State in Frustrated Magnetic Pyrochlore Materials
    journal, November 2001


    Magnetic Coulomb Phase in the Spin Ice Ho2Ti2O7
    journal, September 2009


    The “Coulomb Phase” in Frustrated Systems
    journal, August 2010


    Magnetoelastic excitation spectrum in the rare-earth pyrochlore Tb 2 Ti 2 O 7
    journal, June 2019


    Absence of spin-ice state in the disordered fluorite D y 2 Z r 2 O 7
    journal, June 2019


    Magnetoelastic excitation spectrum in the rare-earth pyrochlore Tb 2 Ti 2 O 7
    journal, June 2019