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

Journal Article · · Physical Review. B, Condensed Matter and Materials Physics
 [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)

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; FG02-08ER46544
OSTI ID:
1213348
Alternate ID(s):
OSTI ID: 1212489
Journal Information:
Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 5; ISSN 1098-0121
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

References (44)

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
Spin fluctuations in the magnetic phase of frustrated pyrochlores: Evidence and controversy journal March 2010
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
Unconventional Anomalous Hall Effect Enhanced by a Noncoplanar Spin Texture in the Frustrated Kondo Lattice Pr 2 Ir 2 O 7 journal January 2007
Zero-and low-field spin relaxation studied by positive muons journal August 1979
Hyperfine interactions-un peu d'histoire journal February 1991
Anisotropic Local Modification of Crystal Field Levels in Pr-Based Pyrochlores: A Muon-Induced Effect Modeled Using Density Functional Theory journal January 2015
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
Electronic changes induced by μ + in PrIn 3 :  Muon-spin-rotation observation and crystalline-electric-field model calculation journal October 1997
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
Investigation of magnetic fluctuations in Tb 2 Sn 2 O 7 ordered spin ice by high-resolution energy-resolved neutron scattering journal November 2008
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
Musrfit: a free platform-independent framework for μSR data analysis text January 2012
Holes in a Quantum Spin Liquid text January 2001
Metal-Nonmetal Changeover in Pyrochlore Iridates text January 2001
Quantal phases, disorder effects and superconductivity in spin-Peierls systems text January 2001
Direct evidence for a dynamical ground state in the highly frustrated Tb$_2$Sn$_2$O$_7$ pyrochlore text January 2006

Cited By (4)

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
Selective probing of magnetic order on Tb and Ir sites in stuffed Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$ using resonant X-ray scattering text January 2019

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