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

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:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1439954