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 »
- Authors:
-
- Univ. of California, Riverside, CA (United States); Univ. of Tokyo, Chiba (Japan)
- California State Univ., Los Angeles, CA (United States)
- Univ. of California, Riverside, CA (United States); Fudan Univ., Shanghai (China)
- Univ. of Tokyo, Chiba (Japan)
- John Hopkins Univ., Baltimore, MD (United States)
- 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)
- 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)
- 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:
- 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. Mon .
"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},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
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}
}
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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
- Kimura, K.; Ohta, Y.; Nakatsuji, S.
- Journal of Physics: Conference Series, Vol. 400, Issue 3
Critical slowing down in the geometrically frustrated pyrochlore antiferromagnet Gd2Ti2O7
journal, March 2006
- MacLaughlin, D. E.; Rose, M. S.; Anderson, J. E.
- Physica B: Condensed Matter, Vol. 374-375
Crystalline electric field levels and magnetic properties of the metallic pyrochlore compound Pr2Ir2O7
journal, August 2005
- Machida, Y.; Nakatsuji, S.; Tonomura, H.
- Journal of Physics and Chemistry of Solids, Vol. 66, Issue 8-9
Low temperature magnetism of the metallic pyrochlore oxide Pr 2+ x Ir 2− x O 7+δ
journal, September 2011
- Kimura, Kenta; Ohta, Yasuo; Nakatsuji, Satoru
- Journal of Physics: Conference Series, Vol. 320
A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source
journal, April 2014
- Stone, M. B.; Niedziela, J. L.; Abernathy, D. L.
- Review of Scientific Instruments, Vol. 85, Issue 4
Muons as probes of dynamical spin fluctuations: some new aspects
journal, September 2004
- Keren, Amit
- Journal of Physics: Condensed Matter, Vol. 16, Issue 40
Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order
journal, December 2009
- Machida, Yo; Nakatsuji, Satoru; Onoda, Shigeki
- Nature, Vol. 463, Issue 7278
Muons and frustrated magnetism in NiGa 2 S 4 and Pr 2 Ir 2 O 7
journal, April 2010
- MacLaughlin, D. E.; Nambu, Y.; Ohta, Y.
- Journal of Physics: Conference Series, Vol. 225
Musrfit: A Free Platform-Independent Framework for μSR Data Analysis
journal, January 2012
- Suter, A.; Wojek, B. M.
- Physics Procedia, Vol. 30
Crystal growth and structure of R2Ir2O7 (R=Pr, Eu) using molten KF
journal, May 2007
- Millican, Jasmine N.; Macaluso, Robin T.; Nakatsuji, Satoru
- Materials Research Bulletin, Vol. 42, Issue 5
Weak quasistatic magnetism in the frustrated Kondo lattice Pr2Ir2O7
journal, April 2009
- MacLaughlin, D. E.; Ohta, Y.; Machida, Y.
- Physica B: Condensed Matter, Vol. 404, Issue 5-7
Disorder, inhomogeneity and spin dynamics in f-electron non-Fermi liquid systems
journal, September 2004
- MacLaughlin, D. E.; Heffner, R. H.; Bernal, O. O.
- Journal of Physics: Condensed Matter, Vol. 16, Issue 40
Spin fluctuations in the magnetic phase of frustrated pyrochlores: Evidence and controversy
journal, March 2010
- Bonville, P.
- Journal of Physics: Conference Series, Vol. 217
Effective hyperfine temperature in frustrated Gd 2Sn 2O 7: two level model and 155Gd Mössbauer measurements
journal, June 2002
- Bertin, E.; Bonville, P.; Bouchard, J. -P.
- The European Physical Journal B - Condensed Matter, Vol. 27, Issue 3, p. 347-354
Metal-Nonmetal Changeover in Pyrochlore Iridates
journal, October 2001
- Yanagishima, Daiki; Maeno, Yoshiteru
- Journal of the Physical Society of Japan, Vol. 70, Issue 10
Metal–Insulator Transition in Pyrochlore Iridates Ln 2 Ir 2 O 7 ( Ln = Nd, Sm, and Eu)
journal, April 2007
- Matsuhira, Kazuyuki; Wakeshima, Makoto; Nakanishi, Ryo
- Journal of the Physical Society of Japan, Vol. 76, Issue 4
Magnetic pyrochlore oxides
journal, January 2010
- Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E.
- Reviews of Modern Physics, Vol. 82, Issue 1
Metallic Spin-Liquid Behavior of the Geometrically Frustrated Kondo Lattice
journal, March 2006
- Nakatsuji, S.; Machida, Y.; Maeno, Y.
- Physical Review Letters, Vol. 96, Issue 8
Unconventional Anomalous Hall Effect Enhanced by a Noncoplanar Spin Texture in the Frustrated Kondo Lattice
journal, January 2007
- Machida, Y.; Nakatsuji, S.; Maeno, Y.
- Physical Review Letters, Vol. 98, Issue 5
Zero-and low-field spin relaxation studied by positive muons
journal, August 1979
- Hayano, R. S.; Uemura, Y. J.; Imazato, J.
- Physical Review B, Vol. 20, Issue 3
Hyperfine interactions-un peu d'histoire
journal, February 1991
- Bleaney, B.
- Hyperfine Interactions, Vol. 63, Issue 1-4
Anisotropic Local Modification of Crystal Field Levels in Pr-Based Pyrochlores: A Muon-Induced Effect Modeled Using Density Functional Theory
journal, January 2015
- Foronda, F. R.; Lang, F.; Möller, J. S.
- Physical Review Letters, Vol. 114, Issue 1
Long-Range Order at Low Temperatures in Dipolar Spin Ice
journal, July 2001
- Melko, Roger G.; den Hertog, Byron C.; Gingras, Michel J. P.
- Physical Review Letters, Vol. 87, Issue 6
Investigation of the Low-Temperature Spin-Liquid Behavior of the Frustrated Magnet Gadolinium Gallium Garnet
journal, May 1998
- Petrenko, O. A.; Ritter, C.; Yethiraj, M.
- Physical Review Letters, Vol. 80, Issue 20
NMR Imaging of the Staggered Magnetization in the Doped Haldane Chain
journal, July 1999
- Tedoldi, F.; Santachiara, R.; Horvatić, M.
- Physical Review Letters, Vol. 83, Issue 2
Quantal Phases, Disorder Effects, and Superconductivity in Spin-Peierls Systems
journal, March 2002
- Tanaka, Akihiro; Hu, Xiao
- Physical Review Letters, Vol. 88, Issue 12
Ordered Spin Ice State and Magnetic Fluctuations in
journal, June 2005
- Mirebeau, I.; Apetrei, A.; Rodríguez-Carvajal, J.
- Physical Review Letters, Vol. 94, Issue 24
Specific Heat of Copper, Silver, and Gold below 30°K
journal, December 1973
- Martin, Douglas L.
- Physical Review B, Vol. 8, Issue 12
Electronic changes induced by in Muon-spin-rotation observation and crystalline-electric-field model calculation
journal, October 1997
- Tashma, T.; Amato, A.; Grayevsky, A.
- Physical Review B, Vol. 56, Issue 15
Probing the Spin-Spin Dynamical Autocorrelation Function in a Spin Glass above via Muon Spin Relaxation
journal, August 1996
- Keren, Amit; Mendels, Philippe; Campbell, Ian A.
- Physical Review Letters, Vol. 77, Issue 7
Magnetic field–time-scaling relations and exotic spin correlations: a μSR study of spin glasses
journal, August 2000
- Keren, Amit; Bazalitsky, Galina; Mendels, Philippe
- Physica B: Condensed Matter, Vol. 289-290
Glassy Spin Dynamics in Non-Fermi-Liquid , 1.0 and 1.5
journal, July 2001
- MacLaughlin, D. E.; Bernal, O. O.; Heffner, R. H.
- Physical Review Letters, Vol. 87, Issue 6
Investigation of magnetic fluctuations in ordered spin ice by high-resolution energy-resolved neutron scattering
journal, November 2008
- Mirebeau, I.; Mutka, H.; Bonville, P.
- Physical Review B, Vol. 78, Issue 17
Spin Dynamics and Magnetic Order in Magnetically Frustrated
journal, March 2006
- Dalmas de Réotier, P.; Yaouanc, A.; Keller, L.
- Physical Review Letters, Vol. 96, Issue 12
Direct Evidence for a Dynamical Ground State in the Highly Frustrated Pyrochlore
journal, September 2006
- Bert, F.; Mendels, P.; Olariu, A.
- Physical Review Letters, Vol. 97, Issue 11
Long-Range Order at Low Temperatures in Dipolar Spin Ice
text, January 2001
- Gingras, Michel J. P.; Melko, Roger G.; Den Hertog, Byron C.
- The American Physical Society
Glassy Spin Dynamics in Non-Fermi-Liquid UCu5xPdx, x = 1.0 and 1.5
text, January 2001
- Bernal, O. O.; Heffner, R. H.; MacLaughlin, D. E.
- The American Physical Society
Musrfit: a free platform-independent framework for μSR data analysis
text, January 2012
- Suter, A.; Wojek, B. M.
- Elsevier
Metal-Nonmetal Changeover in Pyrochlore Iridates
text, January 2001
- Yanagishima, D.; Maeno, Y.
- arXiv
Quantal phases, disorder effects and superconductivity in spin-Peierls systems
text, January 2001
- Tanaka, Akihiro; Hu, Xiao
- arXiv
Direct evidence for a dynamical ground state in the highly frustrated Tb$_2$Sn$_2$O$_7$ pyrochlore
text, January 2006
- Bert, F.; Mendels, P.; Olariu, A.
- arXiv
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
- Ehlers, G.; Podlesnyak, A. A.; Kolesnikov, A. I.
- Review of Scientific Instruments, Vol. 87, Issue 9
Strain-induced spontaneous Hall effect in an epitaxial thin film of a Luttinger semimetal
journal, April 2019
- Ohtsuki, Takumi; Tian, Zhaoming; Endo, Akira
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 18
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
- Donnerer, C.; Rahn, M. C.; Schierle, E.
- Journal of Physics: Condensed Matter, Vol. 31, Issue 34
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
- Donnerer, C.; Rahn, M. C.; Schierle, E.
- arXiv