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Title: Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF 6

Abstract

The Coulomb phase is an idealized state of matter whose properties are determined by factors beyond conventional considerations of symmetry, including global topology, conservation laws and emergent order. In theory, Coulomb phases occur in ice-type systems such as water ice and spin ice; in dimer models; and in certain spin liquids. Yet, apart from ice-type systems, more general experimental examples are very scarce. Here we study the partly disordered material CsNiCrF 6 and show that this material is a multiple Coulomb phase with signature correlations in three degrees of freedom: charge configurations, atom displacements and spin configurations. We use neutron and X-ray scattering to separate these correlations and to determine the magnetic excitation spectrum. Our results reveal how the structural and magnetic properties of apparently disordered materials may inherit, and be dictated by, a hidden symmetry—the local gauge symmetry of an underlying Coulomb phase.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [1];  [4];  [4];  [4];  [1];  [1];  [5]
  1. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  2. Univ. of Edinburgh, Scotland (United Kingdom)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Inst. Laue-Langevin (ILL), Grenoble (France)
  5. Univ. College London (UCL), London (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1506794
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Fennell, T., Harris, M. J., Calder, S., Ruminy, M., Boehm, M., Steffens, P., Lemée-Cailleau, M. -H., Zaharko, O., Cervellino, A., and Bramwell, S. T. Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF6. United States: N. p., 2018. Web. doi:10.1038/s41567-018-0309-3.
Fennell, T., Harris, M. J., Calder, S., Ruminy, M., Boehm, M., Steffens, P., Lemée-Cailleau, M. -H., Zaharko, O., Cervellino, A., & Bramwell, S. T. Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF6. United States. doi:10.1038/s41567-018-0309-3.
Fennell, T., Harris, M. J., Calder, S., Ruminy, M., Boehm, M., Steffens, P., Lemée-Cailleau, M. -H., Zaharko, O., Cervellino, A., and Bramwell, S. T. Mon . "Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF6". United States. doi:10.1038/s41567-018-0309-3. https://www.osti.gov/servlets/purl/1506794.
@article{osti_1506794,
title = {Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF6},
author = {Fennell, T. and Harris, M. J. and Calder, S. and Ruminy, M. and Boehm, M. and Steffens, P. and Lemée-Cailleau, M. -H. and Zaharko, O. and Cervellino, A. and Bramwell, S. T.},
abstractNote = {The Coulomb phase is an idealized state of matter whose properties are determined by factors beyond conventional considerations of symmetry, including global topology, conservation laws and emergent order. In theory, Coulomb phases occur in ice-type systems such as water ice and spin ice; in dimer models; and in certain spin liquids. Yet, apart from ice-type systems, more general experimental examples are very scarce. Here we study the partly disordered material CsNiCrF6 and show that this material is a multiple Coulomb phase with signature correlations in three degrees of freedom: charge configurations, atom displacements and spin configurations. We use neutron and X-ray scattering to separate these correlations and to determine the magnetic excitation spectrum. Our results reveal how the structural and magnetic properties of apparently disordered materials may inherit, and be dictated by, a hidden symmetry—the local gauge symmetry of an underlying Coulomb phase.},
doi = {10.1038/s41567-018-0309-3},
journal = {Nature Physics},
issn = {1745-2473},
number = 1,
volume = 15,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 2 works
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Figures / Tables:

Fig. 1 Fig. 1: Illustration of mappings and structural features of CsNiCrF6. A: The pyrochlore lattice (medial) consists of corner-sharing tetrahedra, on which a Coulomb phase can be established by ensuring that local degrees of freedom can be represented by a non-divergent field that is derived from lattice fluxes on the diamondmore » lattice (parent) (I). A non-divergent configuration of flux variables (blue arrows) around a diamond lattice point is equivalent to the ice rule for spins in a spin ice (two-in-two-out). Antiferromagnetic pseudo-spins are related to the flux variables and configured two-up-two-down in a Coulomb phase ground state (green and orange arrows). B: Two cations occupying the pyrochlore lattice form a charge ice, with cation configurations directly related to the pseudo-spins (green and orange spheres). C: Vector spins coupled antiferromagnetically on the pyrochlore lattice (i.e. a pyrochlore Heisenberg antiferromagnet) must satisfy the condition that the total magnetization of every tetrahedron is zero (black arrows), which can be ensured if the $S$x,y,z vector components are each represented by a family of pseudospins that each obey the ice rule (blue, green and orange arrows). D: In the structure of CsNiCrF6, F- anions (small blue spheres) are coordinated to two cations. The bond valence sum requirements of the cations can be satisfied by displacing anions shared by a pair of unlike cations towards the cation with larger charge (Cr3+). Anions shared between a pair of like cations are not displaced. The edges with non-displaced cations can be identified as a fully packed loop model (FPL) on the diamond lattice, in which loops cover every link of the lattice, every site is visited by exactly two loops, and a given loop is occupied only by one of the cation species (green and orange lines). E: The structure of CsNiCrF6 is composed of the pyrochlore lattice of cations, coordinated by octahedra of F- ions. The octahedra share each of their vertices with one other octahedron, forming tetraheda of tilted octahedra. Extended sections of the FPL are shown, but the octahedra are drawn undistorted. F: The structure contains large cages in which the Cs+ ions reside. The cage coordination is by 18 F- ions, forming an octahedron that is truncated and capped with rectangular pyramids.« less

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Works referenced in this record:

Anharmonic Magnon Excitations in Noncollinear and Charge-Ordered RbFe 2 + Fe 3 + F 6
journal, August 2018


Continuum of quantum fluctuations in a three-dimensional S = 1 Heisenberg magnet
journal, October 2018


The recording and analysis of synchrotron X-radiation Laue diffraction photographs
journal, October 1989

  • Helliwell, J. R.; Habash, J.; Cruickshank, D. W. J.
  • Journal of Applied Crystallography, Vol. 22, Issue 5
  • DOI: 10.1107/S0021889889006564

The Problem with Determining Atomic Structure at the Nanoscale
journal, April 2007


Quantum spin liquids: a review
journal, November 2016


Low-temperature properties of classical geometrically frustrated antiferromagnets
journal, November 1998


Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Coulomb and Liquid Dimer Models in Three Dimensions
journal, October 2003


Emergent excitations in a geometrically frustrated magnet
journal, August 2002


Analysis of a Fully Packed Loop Model Arising in a Magnetic Coulomb Phase
journal, October 2011


Single-crystal diffraction instrument TriCS at SINQ
journal, March 2000


Recent Developments in the Methods and Applications of the Bond Valence Model
journal, December 2009


Seeing the light: Experimental signatures of emergent electromagnetism in a quantum spin ice
journal, August 2012


Dipolar Spin Correlations in Classical Pyrochlore Magnets
journal, October 2004


VIVALDI—A thermal-neutron laue diffractometer for physics, chemistry and materials science
journal, January 2002


Magnetic relaxation in rare-earth oxide pyrochlores
journal, September 2005

  • Ryzhkin, I. A.
  • Journal of Experimental and Theoretical Physics, Vol. 101, Issue 3
  • DOI: 10.1134/1.2103216

Magnetic excitations in a highly frustrated pyrochlore antiferromagnet
journal, July 1995


Properties of a Classical Spin Liquid: The Heisenberg Pyrochlore Antiferromagnet
journal, March 1998


Design of crystal-like aperiodic solids with selective disorder–phonon coupling
journal, February 2016

  • Overy, Alistair R.; Cairns, Andrew B.; Cliffe, Matthew J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10445

Power-law spin correlations in pyrochlore antiferromagnets
journal, January 2005


The Materials Science beamline upgrade at the Swiss Light Source
journal, July 2013

  • Willmott, P. R.; Meister, D.; Leake, S. J.
  • Journal of Synchrotron Radiation, Vol. 20, Issue 5
  • DOI: 10.1107/S0909049513018475

Ordering and Antiferromagnetism in Ferrites
journal, May 1956


Long-Range Order at Low Temperatures in Dipolar Spin Ice
journal, July 2001


Amplitude/Higgs Modes in Condensed Matter Physics
journal, March 2015


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


Spin Dynamics in Pyrochlore Heisenberg Antiferromagnets
journal, June 2009


The use of continuous atomic distributions in structural investigations
journal, September 1994

  • Chernyshev, V. V.; Zhukov, S. G.; Yatsenko, A. V.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 50, Issue 5
  • DOI: 10.1107/S010876739400173X

LAUEGEN version 6.0 and INTLDM
journal, June 1998

  • Campbell, J. W.; Hao, Q.; Harding, M. M.
  • Journal of Applied Crystallography, Vol. 31, Issue 3
  • DOI: 10.1107/S0021889897016683

Short-range magnetic order in the frustrated pyrochlore antiferromagnet CsNiCrF 6
journal, November 1997


Absence of magnetic long-range order in Y 2 CrSbO 7 : Bond-disorder-induced magnetic frustration in a ferromagnetic pyrochlore
journal, September 2017


A short history of SHELX
journal, December 2007

  • Sheldrick, George M.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122
  • DOI: 10.1107/S0108767307043930

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


Disorder-Induced Mimicry of a Spin Liquid in YbMgGaO 4
journal, October 2017


Pyrochlore photons: The U ( 1 ) spin liquid in a S = 1 2 three-dimensional frustrated magnet
journal, February 2004


Random Tiling and Topological Defects in a Two-Dimensional Molecular Network
journal, November 2008


Notizen: Die Struktur einiger Fluoride, Oxide und Oxidfluoride AMe2X6: Der RbNiCrF6-Typ
journal, November 1967

  • Babel, Dietrich; Pausewang, Gerhardt; Viebahn, Werner
  • Zeitschrift für Naturforschung B, Vol. 22, Issue 11
  • DOI: 10.1515/znb-1967-1126

Disordered materials studied using neutron polarization analysis on the multi-detector spectrometer, D7
journal, December 2008

  • Stewart, J. R.; Deen, P. P.; Andersen, K. H.
  • Journal of Applied Crystallography, Vol. 42, Issue 1
  • DOI: 10.1107/S0021889808039162

Atomic displacements in the charge ice pyrochlore Bi 2 Ti 2 O 6 O studied by neutron total scattering
journal, April 2010


Magnetic frustration in the context of pseudo-dipolar ionic disorder
journal, January 2012


Empirical Magnetic Structure Solution of Frustrated Spin Systems
journal, January 2012


Coulombic charge ice
journal, May 2014


Interplay of Superconductivity and Rattling Phenomena in β -Pyrochlore KOs 2 O 6 Studied by Photoemission Spectroscopy
journal, September 2007


Interpretation of diffuse X-ray scattering via models of disorder
journal, June 1994


Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets
journal, May 2014


Geometrical Frustration in the Ferromagnetic Pyrochlore Ho 2 Ti 2 O 7
journal, September 1997


The crystallography of correlated disorder
journal, May 2015


Semiflexible Fully Packed Loop Model and Interacting Rhombus Tilings
journal, April 2009


Magnetic monopoles in spin ice
journal, January 2008

  • Castelnovo, C.; Moessner, R.; Sondhi, S. L.
  • Nature, Vol. 451, Issue 7174
  • DOI: 10.1038/nature06433

Crystalline Electric-Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO 4
journal, March 2017


Breakdown of phonon glass paradigm in La- and Ce-filled Fe4Sb12 skutterudites
journal, August 2008

  • Koza, Michael Marek; Johnson, Mark Robert; Viennois, Romain
  • Nature Materials, Vol. 7, Issue 10
  • DOI: 10.1038/nmat2260

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.