skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Dipolar-octupolar Ising antiferromagnetism in Sm 2 Ti 2 O 7 : A moment fragmentation candidate

Abstract

Over the past two decades, the magnetic ground states of all rare-earth titanate pyrochlores have been extensively studied, with the exception of Sm 2 Ti 2 O 7 . This is, in large part, due to the very high absorption cross section of naturally occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically enriched single crystal of Sm 2 Ti 2 O 7 . Using inelastic neutron scattering, we determine that the crystal field ground state for Sm3+ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm 2 Ti 2 O 7 orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7)μ B below TN=0.35 K, consistent with expectations for antiferromagnetically coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. In conclusion, the combination of the dipolar-octupolar nature of the Sm 3+ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [3];  [4];  [5];  [6];  [6];  [7];  [7];  [8];  [9]; ORCiD logo [3]; ORCiD logo [3];  [10];  [11];  [12]
  1. Univ. of Manitoba, Winnipeg, Manitoba (Canada). Dept. of Chemistry; Univ. of Winnipeg, Winnipeg, Manitoba (Canada). Dept. of Chemistry
  2. McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Rice Univ., Houston, TX (United States). Dept. of Physics and Astronomy and Rice Center for Quantum Materials
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  4. Univ. of Edinburgh, Scotland (United Kingdom). School of Chemistry; Univ. of Edinburgh, Scotland (United Kingdom). Centre for Science at Extreme Conditions
  5. McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
  6. Univ. de Sherbrooke, Sherbrooke, Québec (Canada). Inst. Quantique and Dépt. de Physique
  7. Univ. of Manitoba, Winnipeg, Manitoba (Canada). Dept. of Chemistry
  8. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  9. Inst. Laue-Langevin, Grenoble (France)
  10. McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Canadian Inst. for Advanced Research, Toronto, Ontario (Canada); TRIUMF, Vancouver, BC (Canada)
  11. McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Canadian Inst. for Advanced Research, Toronto, Ontario (Canada)
  12. Univ. of Manitoba, Winnipeg, Manitoba (Canada). Dept. of Chemistry; Univ. of Winnipeg, Winnipeg, Manitoba (Canada). Dept. of Chemistry; McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Canadian Inst. for Advanced Research, Toronto, Ontario (Canada)
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:
1470878
Alternate Identifier(s):
OSTI ID: 1468836
Grant/Contract Number:  
[AC05-00OR22725]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
[ Journal Volume: 98; Journal Issue: 10]; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Mauws, Cole, Hallas, A. M., Sala, Gabriele, Aczel, Adam A., Sarte, P. M., Gaudet, J., Ziat, D., Quilliam, J. A., Lussier, J. A., Bieringer, M., Zhou, H. D., Wildes, A., Stone, Matthew B., Abernathy, Douglas L., Luke, G. M., Gaulin, B. D., and Wiebe, Christopher R. Dipolar-octupolar Ising antiferromagnetism in Sm2Ti2O7 : A moment fragmentation candidate. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.98.100401.
Mauws, Cole, Hallas, A. M., Sala, Gabriele, Aczel, Adam A., Sarte, P. M., Gaudet, J., Ziat, D., Quilliam, J. A., Lussier, J. A., Bieringer, M., Zhou, H. D., Wildes, A., Stone, Matthew B., Abernathy, Douglas L., Luke, G. M., Gaulin, B. D., & Wiebe, Christopher R. Dipolar-octupolar Ising antiferromagnetism in Sm2Ti2O7 : A moment fragmentation candidate. United States. doi:10.1103/PhysRevB.98.100401.
Mauws, Cole, Hallas, A. M., Sala, Gabriele, Aczel, Adam A., Sarte, P. M., Gaudet, J., Ziat, D., Quilliam, J. A., Lussier, J. A., Bieringer, M., Zhou, H. D., Wildes, A., Stone, Matthew B., Abernathy, Douglas L., Luke, G. M., Gaulin, B. D., and Wiebe, Christopher R. Wed . "Dipolar-octupolar Ising antiferromagnetism in Sm2Ti2O7 : A moment fragmentation candidate". United States. doi:10.1103/PhysRevB.98.100401. https://www.osti.gov/servlets/purl/1470878.
@article{osti_1470878,
title = {Dipolar-octupolar Ising antiferromagnetism in Sm2Ti2O7 : A moment fragmentation candidate},
author = {Mauws, Cole and Hallas, A. M. and Sala, Gabriele and Aczel, Adam A. and Sarte, P. M. and Gaudet, J. and Ziat, D. and Quilliam, J. A. and Lussier, J. A. and Bieringer, M. and Zhou, H. D. and Wildes, A. and Stone, Matthew B. and Abernathy, Douglas L. and Luke, G. M. and Gaulin, B. D. and Wiebe, Christopher R.},
abstractNote = {Over the past two decades, the magnetic ground states of all rare-earth titanate pyrochlores have been extensively studied, with the exception of Sm2Ti2O7. This is, in large part, due to the very high absorption cross section of naturally occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically enriched single crystal of Sm2Ti2O7. Using inelastic neutron scattering, we determine that the crystal field ground state for Sm3+ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm2Ti2O7 orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7)μB below TN=0.35 K, consistent with expectations for antiferromagnetically coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. In conclusion, the combination of the dipolar-octupolar nature of the Sm3+ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics.},
doi = {10.1103/PhysRevB.98.100401},
journal = {Physical Review B},
number = [10],
volume = [98],
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions
journal, March 1952


Pyrochlores. V. Thermoanalytic, X-ray, neutron, infrared, and dielectric studies of A 2 Ti 2 O 7 titanates
journal, March 1969

  • Knop, Osvald; Brisse, François; Castelliz, Lotte
  • Canadian Journal of Chemistry, Vol. 47, Issue 6
  • DOI: 10.1139/v69-155

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

Observation of long-range magnetic ordering in pyrohafnate Nd 2 Hf 2 O 7 : A neutron diffraction study
journal, November 2015


Nd 2 Sn 2 O 7 : An all-in–all-out pyrochlore magnet with no divergence-free field and anomalously slow paramagnetic spin dynamics
journal, October 2015


SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010


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


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


Zero-point entropy in ‘spin ice’
journal, May 1999

  • Ramirez, A. P.; Hayashi, A.; Cava, R. J.
  • Nature, Vol. 399, Issue 6734
  • DOI: 10.1038/20619

Observation of magnetic fragmentation in spin ice
journal, April 2016

  • Petit, S.; Lhotel, E.; Canals, B.
  • Nature Physics, Vol. 12, Issue 8
  • DOI: 10.1038/nphys3710

Quantum Spin Ices and Topological Phases from Dipolar-Octupolar Doublets on the Pyrochlore Lattice
journal, April 2014


Magnetic-Moment Fragmentation and Monopole Crystallization
journal, January 2014


Static magnetic susceptibility, crystal field and exchange interactions in rare earth titanate pyrochlores
journal, June 2010

  • Malkin, B. Z.; Lummen, T. T. A.; van Loosdrecht, P. H. M.
  • Journal of Physics: Condensed Matter, Vol. 22, Issue 27
  • DOI: 10.1088/0953-8984/22/27/276003

Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd 2 Zr 2 O 7
journal, December 2015


Crystal field states of Tb 3 + in the pyrochlore spin liquid Tb 2 Ti 2 O 7 from neutron spectroscopy
journal, June 2015


Treating crystal field parameters in lower than cubic symmetries
journal, January 1984


Theory of Spin-Orbit Coupling in Atoms. III
journal, April 1964


Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7
journal, May 2000

  • Rosenkranz, S.; Ramirez, A. P.; Hayashi, A.
  • Journal of Applied Physics, Vol. 87, Issue 9
  • DOI: 10.1063/1.372565

Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012

  • Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
  • Review of Scientific Instruments, Vol. 83, Issue 1
  • DOI: 10.1063/1.3680104

Fluctuations and All-In–All-Out Ordering in Dipole-Octupole Nd 2 Zr 2 O 7
journal, November 2015


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


Quantum origins of moment fragmentation in Nd 2 Zr 2 O 7
journal, September 2016


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


Crystal electric field in the R 2 Ti 2 O 7 pyrochlore compounds
journal, May 2012


Manifestation of geometric frustration on magnetic and thermodynamic properties of the pyrochlores Sm 2 X 2 O 7 ( X = Ti , Zr )
journal, February 2008


Crystal-field parameters of the rare-earth pyrochlores R 2 Ti 2 O 7 ( R = Tb , Dy, and Ho)
journal, July 2016


Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb 2 Ti 2 O 7
journal, October 2015


Effect of chemical pressure on the crystal electric field states of erbium pyrochlore magnets
journal, January 2018


MCViNE – An object oriented Monte Carlo neutron ray tracing simulation package
journal, February 2016

  • Lin, Jiao Y. Y.; Smith, Hillary L.; Granroth, Garrett E.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 810
  • DOI: 10.1016/j.nima.2015.11.118