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Title: Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er 2 Ge 2 O 7

Abstract

The recent discoveries of proximate quantum spin-liquid compounds and their potential application in quantum computing informs the search for new candidate materials for quantum spin-ice and spin-liquid physics. While the majority of such work has centered on members of the pyrochlore family due to their inherently frustrated linked tetrahedral structure, the rare-earth pyrogermanates also show promise for possible frustrated magnetic behavior. With the familiar stoichiometry R2Ge2O7, these compounds generally have tetragonal symmetry with a rare-earth sublattice built of a spiral of alternating edge and corner-sharing rare-earth site triangles. Studies on Dy2Ge2O7 and Ho2Ge2O7 have shown tunable low temperature antiferromagnetic order, a high frustration index, and spin-ice-like dynamics. Here we use neutron diffraction to study magnetic order in Er2Ge2O7 (space group P41212) and find the lowest yet Neél temperature in the pyrogermanates of 1.15 K. Using neutron powder diffraction, we find the magnetic structure to order with k=(0,0,0) ordering vector, magnetic space group symmetry P4'1212', and a refined Er moment of m=8.1μB near the expected value for the Er3+ free ion. Provocatively, the magnetic structure exhibits similar “local Ising” behavior to that seen in the pyrocholres where the Er moment points up or down along the short Er-Er bond. Upon applyingmore » a magnetic field, we find a first-order metamagnetic transition at ~0.35T to a lower symmetry P2'12'12 structure. This magnetic transition involves an inversion of Er moments aligned antiparallel to the applied field describing a class I spin-flip-type transition, indicating a strong local anisotropy at the Er site—reminiscent of that seen in the spin-ice pyrochlores.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Clemson Univ., SC (United States). Dept. of Chemistry
  3. Clemson Univ., SC (United States). Dept. of Chemistry
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Clemson Univ., SC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1490717
Alternate Identifier(s):
OSTI ID: 1490561; OSTI ID: 1596457
Grant/Contract Number:  
AC05-00OR22725; SC0014271
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; hydrothermal single crystals erbium tetragonal germinate

Citation Formats

Taddei, Keith M., Sanjeewa, Liurukara D., Kolis, Joseph W., Sefat, Athena Safa, Dela Cruz, Clarina R., and Pajerowski, Daniel M. Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er2Ge2O7. United States: N. p., 2019. Web. doi:10.1103/physrevmaterials.3.014405.
Taddei, Keith M., Sanjeewa, Liurukara D., Kolis, Joseph W., Sefat, Athena Safa, Dela Cruz, Clarina R., & Pajerowski, Daniel M. Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er2Ge2O7. United States. https://doi.org/10.1103/physrevmaterials.3.014405
Taddei, Keith M., Sanjeewa, Liurukara D., Kolis, Joseph W., Sefat, Athena Safa, Dela Cruz, Clarina R., and Pajerowski, Daniel M. Fri . "Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er2Ge2O7". United States. https://doi.org/10.1103/physrevmaterials.3.014405. https://www.osti.gov/servlets/purl/1490717.
@article{osti_1490717,
title = {Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er2Ge2O7},
author = {Taddei, Keith M. and Sanjeewa, Liurukara D. and Kolis, Joseph W. and Sefat, Athena Safa and Dela Cruz, Clarina R. and Pajerowski, Daniel M.},
abstractNote = {The recent discoveries of proximate quantum spin-liquid compounds and their potential application in quantum computing informs the search for new candidate materials for quantum spin-ice and spin-liquid physics. While the majority of such work has centered on members of the pyrochlore family due to their inherently frustrated linked tetrahedral structure, the rare-earth pyrogermanates also show promise for possible frustrated magnetic behavior. With the familiar stoichiometry R2Ge2O7, these compounds generally have tetragonal symmetry with a rare-earth sublattice built of a spiral of alternating edge and corner-sharing rare-earth site triangles. Studies on Dy2Ge2O7 and Ho2Ge2O7 have shown tunable low temperature antiferromagnetic order, a high frustration index, and spin-ice-like dynamics. Here we use neutron diffraction to study magnetic order in Er2Ge2O7 (space group P41212) and find the lowest yet Neél temperature in the pyrogermanates of 1.15 K. Using neutron powder diffraction, we find the magnetic structure to order with k=(0,0,0) ordering vector, magnetic space group symmetry P4'1212', and a refined Er moment of m=8.1μB near the expected value for the Er3+ free ion. Provocatively, the magnetic structure exhibits similar “local Ising” behavior to that seen in the pyrocholres where the Er moment points up or down along the short Er-Er bond. Upon applying a magnetic field, we find a first-order metamagnetic transition at ~0.35T to a lower symmetry P2'12'12 structure. This magnetic transition involves an inversion of Er moments aligned antiparallel to the applied field describing a class I spin-flip-type transition, indicating a strong local anisotropy at the Er site—reminiscent of that seen in the spin-ice pyrochlores.},
doi = {10.1103/physrevmaterials.3.014405},
journal = {Physical Review Materials},
number = 1,
volume = 3,
place = {United States},
year = {Fri Jan 11 00:00:00 EST 2019},
month = {Fri Jan 11 00:00:00 EST 2019}
}

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Works referenced in this record:

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016

  • Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
  • Nature Materials, Vol. 15, Issue 7
  • DOI: 10.1038/nmat4604

Spin liquids in frustrated magnets
journal, March 2010


Antiferromagnetism. The Triangular Ising Net
journal, July 1950


Phase transitions in a programmable quantum spin glass simulator
journal, July 2018


How ‘spin ice’ freezes
journal, September 2001

  • Snyder, J.; Slusky, J. S.; Cava, R. J.
  • Nature, Vol. 413, Issue 6851
  • DOI: 10.1038/35092516

Magnetic pyrochlore oxides
journal, January 2010

  • Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E.
  • Reviews of Modern Physics, Vol. 82, Issue 1
  • DOI: 10.1103/RevModPhys.82.53

Pronounced first-order metamagnetic transition in the paramagnetic heavy-fermion system CeTiGe
journal, February 2012


Measurements of magnetic susceptibilities and anisotropy of erbium pyrogermanate (Er2Ge2O7) crystal
journal, May 1998


Physical realization of a quantum spin liquid based on a complex frustration mechanism
journal, July 2016

  • Balz, Christian; Lake, Bella; Reuther, Johannes
  • Nature Physics, Vol. 12, Issue 10
  • DOI: 10.1038/nphys3826

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976


Neutron scattering in the proximate quantum spin liquid α-RuCl 3
journal, June 2017


Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets
journal, April 2000


Quantum Spin Liquid from a Three-Dimensional Copper-Oxalate Framework
journal, December 2017

  • Zhang, Bin; Baker, Peter J.; Zhang, Yan
  • Journal of the American Chemical Society, Vol. 140, Issue 1
  • DOI: 10.1021/jacs.7b11179

Magnetization curve of spin ice in a [111] magnetic field
journal, September 2004


Ising versus X Y Anisotropy in Frustrated R 2 Ti 2 O 7 Compounds as “Seen” by Polarized Neutrons
journal, July 2009


Field-Induced Spin-Ice-Like Orders in Spin Liquid Tb 2 Ti 2 O 7
journal, November 2008


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


Magnetic anisotropy of the spin-ice compound Dy2Ti2O7
journal, January 2002


Magnetothermodynamics of the Ising antiferromagnet Dy 2 Ge 2 O 7
journal, September 2008


First Order Metamagnetic Transition in Ho 2 Ti 2 O 7 Observed by Vibrating Coil Magnetometry at Milli-Kelvin Temperatures
journal, June 2012


Frustrated rare earth magnetism: Spin glasses, spin liquids and spin ices in pyrochlore oxides
journal, February 2006


Crystal structure refinement with SHELXL
journal, January 2015

  • Sheldrick, George M.
  • Acta Crystallographica Section C Structural Chemistry, Vol. 71, Issue 1, p. 3-8
  • DOI: 10.1107/S2053229614024218

Magnetic form Factors
journal, December 1982


VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011


Field-induced metamagnetic transitions and two-dimensional excitations in ludwigite Co 4 . 76 Al 1 . 24 ( O 2 BO 3 ) 2
journal, June 2017


Majorana fermions in the Kitaev quantum spin system α-RuCl3
journal, September 2017

  • Do, Seung-Hwan; Park, Sang-Youn; Yoshitake, Junki
  • Nature Physics, Vol. 13, Issue 11
  • DOI: 10.1038/nphys4264

Majorana fermions in condensed matter: An outlook
journal, May 2017


Simple frustrated systems: chains, strips and squares
journal, December 1978

  • Derrida, B.; Vannimenus, J.; Pomeau, Y.
  • Journal of Physics C: Solid State Physics, Vol. 11, Issue 23
  • DOI: 10.1088/0022-3719/11/23/019

Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α RuCl 3
journal, December 2017


Metamagnetism
journal, September 1977


Phases and structural relations of the rare earth germanates RE2Ge2O7, RE ≡ La-Lu
journal, February 1987


Low-temperature spin freezing in the Dy 2 Ti 2 O 7 spin ice
journal, February 2004


Fault-tolerant quantum computation by anyons
journal, January 2003


Specific Heat of Kagomé Ice in the Pyrochlore Oxide Dy 2 Ti 2 O 7
journal, February 2003

  • Hiroi, Zenji; Matsuhira, Kazuyuki; Takagi, Seishi
  • Journal of the Physical Society of Japan, Vol. 72, Issue 2
  • DOI: 10.1143/JPSJ.72.411

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


Frustration in Ising-type spin models on the pyrochlore lattice
journal, April 1998


A correction for powder diffraction peak asymmetry due to axial divergence
journal, December 1994

  • Finger, L. W.; Cox, D. E.; Jephcoat, A. P.
  • Journal of Applied Crystallography, Vol. 27, Issue 6
  • DOI: 10.1107/S0021889894004218

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


ISODISPLACE : a web-based tool for exploring structural distortions
journal, July 2006

  • Campbell, Branton J.; Stokes, Harold T.; Tanner, David E.
  • Journal of Applied Crystallography, Vol. 39, Issue 4
  • DOI: 10.1107/S0021889806014075

Magnetization Process of a Screw Spin System. II
journal, January 1964

  • Kitano, Yoshiharu; Nagamiya, Takeo
  • Progress of Theoretical Physics, Vol. 31, Issue 1
  • DOI: 10.1143/PTP.31.1

Candidate quantum spin ice in the pyrochlore Pr 2 Hf 2 O 7
journal, July 2016


Structure and magnetic properties of the Ho 2 Ge 2 O 7 pyrogermanate
journal, June 2008


Strongly Geometrically Frustrated Magnets
journal, August 1994


Magnetic monopoles in spin ice
journal, January 2008

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

Ising Pyrochlore Magnets: Low-Temperature Properties, “Ice Rules,” and Beyond
journal, August 1999


Evidence for two distinct spin relaxation mechanisms in  hot  spin ice Ho 2 Ti 2 O 7
journal, March 2004


Strongly Geometrically Frustrated Magnets
journal, January 1994


Lead palladium titanate: A room temperature nanoscale multiferroic thin film
journal, February 2020


Antiferromagnetism. The Triangular Ising Net
journal, June 1973


Magnetic Monopoles in Spin Ice
journal, January 2008


Neutron scattering in the proximate quantum spin liquid α-RuCl3.
text, January 2017

  • Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.11028

Field induced spin ice like orders in spin liquid Tb$_2$Ti$_2$O$_7$
text, January 2008


Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets
text, January 2000


Ising pyrochlore magnets: Low temperature properties, ice rules and beyond
text, January 1999