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

Title: Unstable spin-ice order in the stuffed metallic pyrochlore Pr2+xIr2-xO7-δ

Abstract

Specific heat, elastic neutron scattering, and muon spin rotation experiments have been carried out on a well-characterized sample of “stuffed” (Pr-rich) Pr2+xIr2-xO7-δ. Elastic neutron scattering shows the onset of long-range spin-ice “2-in/2-out” magnetic order at 0.93 kelvin, with an ordered moment of 1.7(1) Bohr magnetons per Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 angstroms and 0.7 nanosecond, respectively. Muon spin rotation experiments yield an upper bound 2.6(7) milliteslas on the local field B4floc at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7-Bohr magneton moments (120–270 milliteslas, depending on the muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr3+ ions by the positive-muon-induced lattice distortion. For this to be the only effect, however, ~160 Pr moments out to a distance of ~14 angstroms must be suppressed. An alternative scenario—one consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat—invokes slow correlated Pr-moment fluctuations in the ordered state that average B4floc on the μSR time scale (~10-7 second), but are staticmore » on the time scale of the elastic neutron scattering experiments (~10-9 second). In this picture, the dynamic muon relaxation suggests a Pr3+ 4f correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.« less

Authors:
 [1];  [2];  [3];  [4];  [4];  [5];  [5];  [6];  [7];  [8];  [4];  [4];  [9];  [4];  [4]
  1. Univ. of California, Riverside, CA (United States); Univ. of Tokyo, Chiba (Japan)
  2. California State Univ., Los Angeles, CA (United States)
  3. Univ. of California, Riverside, CA (United States); Fudan Univ., Shanghai (China)
  4. Univ. of Tokyo, Chiba (Japan)
  5. John Hopkins Univ., Baltimore, MD (United States)
  6. John Hopkins Univ., Baltimore, MD (United States); National Institute of Standards and Technology, Gaithersburg, MD (United States)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  8. John Hopkins Univ., Baltimore, MD (United States); National Institute of Standards and Technology, Gaithersburg, MD (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  9. Univ. of Tokyo, Chiba (Japan); Japan Science and Technology Agency, Saitama (Japan)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1213348
Alternate Identifier(s):
OSTI ID: 1212489
Grant/Contract Number:  
AC05-00OR22725; FG02-08ER46544
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 5; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

MacLaughlin, D. E., Bernal, O. O., Shu, Lei, Ishikawa, Jun, Matsumoto, Yosuke, Wen, Jia -Jia, Mourigal, Martin P., Stock, C., Ehlers, Georg, Broholm, C. L., Machida, Yo, Kimura, Kenta, Nakatsuji, Satoru, Shimura, Yasuyuki, and Sakakibara, Toshiro. Unstable spin-ice order in the stuffed metallic pyrochlore Pr2+xIr2-xO7-δ. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.054432.
MacLaughlin, D. E., Bernal, O. O., Shu, Lei, Ishikawa, Jun, Matsumoto, Yosuke, Wen, Jia -Jia, Mourigal, Martin P., Stock, C., Ehlers, Georg, Broholm, C. L., Machida, Yo, Kimura, Kenta, Nakatsuji, Satoru, Shimura, Yasuyuki, & Sakakibara, Toshiro. Unstable spin-ice order in the stuffed metallic pyrochlore Pr2+xIr2-xO7-δ. United States. https://doi.org/10.1103/PhysRevB.92.054432
MacLaughlin, D. E., Bernal, O. O., Shu, Lei, Ishikawa, Jun, Matsumoto, Yosuke, Wen, Jia -Jia, Mourigal, Martin P., Stock, C., Ehlers, Georg, Broholm, C. L., Machida, Yo, Kimura, Kenta, Nakatsuji, Satoru, Shimura, Yasuyuki, and Sakakibara, Toshiro. 2015. "Unstable spin-ice order in the stuffed metallic pyrochlore Pr2+xIr2-xO7-δ". United States. https://doi.org/10.1103/PhysRevB.92.054432. https://www.osti.gov/servlets/purl/1213348.
@article{osti_1213348,
title = {Unstable spin-ice order in the stuffed metallic pyrochlore Pr2+xIr2-xO7-δ},
author = {MacLaughlin, D. E. and Bernal, O. O. and Shu, Lei and Ishikawa, Jun and Matsumoto, Yosuke and Wen, Jia -Jia and Mourigal, Martin P. and Stock, C. and Ehlers, Georg and Broholm, C. L. and Machida, Yo and Kimura, Kenta and Nakatsuji, Satoru and Shimura, Yasuyuki and Sakakibara, Toshiro},
abstractNote = {Specific heat, elastic neutron scattering, and muon spin rotation experiments have been carried out on a well-characterized sample of “stuffed” (Pr-rich) Pr2+xIr2-xO7-δ. Elastic neutron scattering shows the onset of long-range spin-ice “2-in/2-out” magnetic order at 0.93 kelvin, with an ordered moment of 1.7(1) Bohr magnetons per Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 angstroms and 0.7 nanosecond, respectively. Muon spin rotation experiments yield an upper bound 2.6(7) milliteslas on the local field B4floc at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7-Bohr magneton moments (120–270 milliteslas, depending on the muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr3+ ions by the positive-muon-induced lattice distortion. For this to be the only effect, however, ~160 Pr moments out to a distance of ~14 angstroms must be suppressed. An alternative scenario—one consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat—invokes slow correlated Pr-moment fluctuations in the ordered state that average B4floc on the μSR time scale (~10-7 second), but are static on the time scale of the elastic neutron scattering experiments (~10-9 second). In this picture, the dynamic muon relaxation suggests a Pr3+ 4f correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.},
doi = {10.1103/PhysRevB.92.054432},
url = {https://www.osti.gov/biblio/1213348}, journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 5,
volume = 92,
place = {United States},
year = {Mon Aug 24 00:00:00 EDT 2015},
month = {Mon Aug 24 00:00:00 EDT 2015}
}

Journal Article:

Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Structural, Magnetic, and Electrical Properties in the Metallic Pyrochlore Pr 2+ x Ir 2- x O 7+ δ
journal, December 2012


Critical slowing down in the geometrically frustrated pyrochlore antiferromagnet Gd2Ti2O7
journal, March 2006


Enhanced nuclear magnetism
journal, October 1973


Crystalline electric field levels and magnetic properties of the metallic pyrochlore compound Pr2Ir2O7
journal, August 2005


Low temperature magnetism of the metallic pyrochlore oxide Pr 2+ x Ir 2− x O 7+δ
journal, September 2011


A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source
journal, April 2014


Muons as probes of dynamical spin fluctuations: some new aspects
journal, September 2004


Holes in a Quantum Spin Liquid
journal, July 2000


Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order
journal, December 2009


Muons and frustrated magnetism in NiGa 2 S 4 and Pr 2 Ir 2 O 7
journal, April 2010


Musrfit: A Free Platform-Independent Framework for μSR Data Analysis
journal, January 2012


Crystal growth and structure of R2Ir2O7 (R=Pr, Eu) using molten KF
journal, May 2007


Weak quasistatic magnetism in the frustrated Kondo lattice Pr2Ir2O7
journal, April 2009


Disorder, inhomogeneity and spin dynamics in f-electron non-Fermi liquid systems
journal, September 2004


Effective hyperfine temperature in frustrated Gd 2Sn 2O 7: two level model and 155Gd Mössbauer measurements
journal, June 2002


Metal-Nonmetal Changeover in Pyrochlore Iridates
journal, October 2001


Metal–Insulator Transition in Pyrochlore Iridates Ln 2 Ir 2 O 7 ( Ln = Nd, Sm, and Eu)
journal, April 2007


Magnetic pyrochlore oxides
journal, January 2010


Metallic Spin-Liquid Behavior of the Geometrically Frustrated Kondo Lattice Pr 2 Ir 2 O 7
journal, March 2006


Zero-and low-field spin relaxation studied by positive muons
journal, August 1979


Hyperfine interactions-un peu d'histoire
journal, February 1991


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


Investigation of the Low-Temperature Spin-Liquid Behavior of the Frustrated Magnet Gadolinium Gallium Garnet
journal, May 1998


Y 89 NMR Imaging of the Staggered Magnetization in the Doped Haldane Chain Y 2 BaNi 1 x Mg x O 5
journal, July 1999


Quantal Phases, Disorder Effects, and Superconductivity in Spin-Peierls Systems
journal, March 2002


Ordered Spin Ice State and Magnetic Fluctuations in Tb 2 Sn 2 O 7
journal, June 2005


Specific Heat of Copper, Silver, and Gold below 30°K
journal, December 1973


Probing the Spin-Spin Dynamical Autocorrelation Function in a Spin Glass above T g via Muon Spin Relaxation
journal, August 1996


Magnetic field–time-scaling relations and exotic spin correlations: a μSR study of spin glasses
journal, August 2000


Glassy Spin Dynamics in Non-Fermi-Liquid UCu 5 x Pd x , x = 1.0 and 1.5
journal, July 2001


Spin Dynamics and Magnetic Order in Magnetically Frustrated Tb 2 Sn 2 O 7
journal, March 2006


Direct Evidence for a Dynamical Ground State in the Highly Frustrated Tb 2 Sn 2 O 7 Pyrochlore
journal, September 2006


Long-Range Order at Low Temperatures in Dipolar Spin Ice
text, January 2001


Glassy Spin Dynamics in Non-Fermi-Liquid UCu5–xPdx, x = 1.0 and 1.5
text, January 2001


Holes in a Quantum Spin Liquid
text, January 2001


Works referencing / citing this record:

The cold neutron chopper spectrometer at the Spallation Neutron Source—A review of the first 8 years of operation
journal, September 2016


Strain-induced spontaneous Hall effect in an epitaxial thin film of a Luttinger semimetal
journal, April 2019


Selective probing of magnetic order on Tb and Ir sites in stuffed Tb 2 Ir 2 O 7  using resonant x-ray scattering
journal, June 2019