Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd2Zr2O7

Xu, J.; Anand, V. K.; Bera, A. K.; Frontzek, Matthias D.; Abernathy, Douglas L.; Casati, N.; Siemensmeyer, K.; Lake, B.

doi:10.1103/PhysRevB.92.224430

Title: Magnetic structure and crystal-field states of the pyrochlore antiferromagnet ${Nd}_{2} {Zr}_{2} O_{7}$

Journal Article · Mon Dec 28 00:00:00 EST 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.92.224430· OSTI ID:1311258

Xu, J. ^[1]; Anand, V. K. ^[2]; Bera, A. K. ^[3]; Frontzek, Matthias D. ^[4]; Abernathy, Douglas L. ^[5]; Casati, N. ^[4]; Siemensmeyer, K. ^[2]; Lake, B. ^[1]

Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany); Technische Univ. Berlin (Germany)
Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany)
Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany); Bhabha Atomic Research Centre (BARC), Mumbai (India)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this paper, we present synchrotron x-ray diffraction, neutron powder diffraction, and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd₂Zr₂O₇ to study the ordered state magnetic structure and cystal-field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long-range all-in/all-out antiferromagnetic order below T_N≈0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) μ_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65μ_B/Nd for the local <111> Ising ground state of Nd³⁺ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The inelastic neutron scattering experiment further confirms the Ising anisotropic ground state of Nd³⁺ and also reveals its dipolar-octupolar character which possibly induces the quantum fluctuation. Lastly, the crystal-field level scheme and ground state wave function have been determined.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Helmholtz Virtual Institute

Grant/Contract Number:: AC05-00OR22725; VHVI-521

OSTI ID:: 1311258

Alternate ID(s):: OSTI ID: 1234009

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 22; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 68 works

Citation information provided by
Web of Science

References (49)

Introduction to Frustrated Magnetism Lacroix, Claudine; Mendels, Philippe; Mila, Frédéric Springer Series in Solid-State Sciences https://doi.org/10.1007/978-3-642-10589-0	book	January 2011
Magnetic pyrochlore oxides Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E. Reviews of Modern Physics, Vol. 82, Issue 1 https://doi.org/10.1103/RevModPhys.82.53	journal	January 2010
Chemical pressure effects on magnetism in the quantum spin liquid candidates Yb $_{2} X_{2}$ O $_{7}$ ( $X = Sn$ , Ti, Ge) Dun, Z. L.; Lee, M.; Choi, E. S. Physical Review B, Vol. 89, Issue 6 https://doi.org/10.1103/PhysRevB.89.064401	journal	February 2014
Magnetic monopoles in spin ice Castelnovo, C.; Moessner, R.; Sondhi, S. L. Nature, Vol. 451, Issue 7174 https://doi.org/10.1038/nature06433	journal	January 2008
Dirac Strings and Magnetic Monopoles in the Spin Ice Dy2Ti2O7 Morris, D. J. P.; Tennant, D. A.; Grigera, S. A. Science, Vol. 326, Issue 5951 https://doi.org/10.1126/science.1178868	journal	September 2009
Magnetic Coulomb Phase in the Spin Ice Ho2Ti2O7 Fennell, T.; Deen, P. P.; Wildes, A. R. Science, Vol. 326, Issue 5951 https://doi.org/10.1126/science.1177582	journal	September 2009
Long-range order and spin-liquid states of polycrystalline Tb $_{2 + x}$ Ti $_{2 - x}$ O $_{7 + y}$ Taniguchi, T.; Kadowaki, H.; Takatsu, H. Physical Review B, Vol. 87, Issue 6 https://doi.org/10.1103/PhysRevB.87.060408	journal	February 2013
${Er}_{2} {Ti}_{2} O_{7} :$ Evidence of quantum order by disorder in a frustrated antiferromagnet Champion, J. D. M.; Harris, M. J.; Holdsworth, P. C. W. Physical Review B, Vol. 68, Issue 2 https://doi.org/10.1103/PhysRevB.68.020401	journal	July 2003
Monte Carlo studies of the dipolar spin ice model Melko, Roger G.; Gingras, Michel J. P. Journal of Physics: Condensed Matter, Vol. 16, Issue 43 https://doi.org/10.1088/0953-8984/16/43/R02	journal	October 2004
Magnetic-Moment Fragmentation and Monopole Crystallization Brooks-Bartlett, M. E.; Banks, S. T.; Jaubert, L. D. C. Physical Review X, Vol. 4, Issue 1 https://doi.org/10.1103/PhysRevX.4.011007	journal	January 2014
Monopole ordered phases in dipolar and nearest-neighbors Ising pyrochlore: From spin ice to the all-in–all-out antiferromagnet Guruciaga, P. C.; Grigera, S. A.; Borzi, R. A. Physical Review B, Vol. 90, Issue 18 https://doi.org/10.1103/PhysRevB.90.184423	journal	November 2014
Quantum Spin Ices and Topological Phases from Dipolar-Octupolar Doublets on the Pyrochlore Lattice Huang, Yi-Ping; Chen, Gang; Hermele, Michael Physical Review Letters, Vol. 112, Issue 16 https://doi.org/10.1103/PhysRevLett.112.167203	journal	April 2014
Emergence of Magnetic Long-range Order in Frustrated Pyrochlore Nd ₂ Ir ₂ O ₇ with Metal–Insulator Transition Tomiyasu, Keisuke; Matsuhira, Kazuyuki; Iwasa, Kazuaki Journal of the Physical Society of Japan, Vol. 81, Issue 3 https://doi.org/10.1143/JPSJ.81.034709	journal	March 2012
Magnetic order in the pyrochlore iridate Nd $_{2}$ Ir $_{2}$ O $_{7}$ probed by muon spin relaxation Guo, Hanjie; Matsuhira, Kazuyuki; Kawasaki, Ikuto Physical Review B, Vol. 88, Issue 6 https://doi.org/10.1103/PhysRevB.88.060411	journal	August 2013
Magnetic Structure of Nd ₂ Mo ₂ O ₇ Yasui, Yukio; Kondo, Yasuyuki; Kanada, Masaki Journal of the Physical Society of Japan, Vol. 70, Issue 1 https://doi.org/10.1143/JPSJ.70.284	journal	January 2001
Neutron Scattering Studies of Pyrochlore Compound Nd ₂ Mo ₂ O ₇ in Magnetic Field Yasui, Yukio; Iikubo, Satoshi; Harashina, Hiroshi Journal of the Physical Society of Japan, Vol. 72, Issue 4 https://doi.org/10.1143/JPSJ.72.865	journal	April 2003
${Nd}_{2} {Sn}_{2} O_{7}$ : An all-in–all-out pyrochlore magnet with no divergence-free field and anomalously slow paramagnetic spin dynamics Bertin, A.; Dalmas de Réotier, P.; Fåk, B. Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.144423	journal	October 2015
Observation of long-range magnetic ordering in pyrohafnate ${Nd}_{2} {Hf}_{2} O_{7}$ : A neutron diffraction study Anand, V. K.; Bera, A. K.; Xu, J. Physical Review B, Vol. 92, Issue 18 https://doi.org/10.1103/PhysRevB.92.184418	journal	November 2015
Heat-capacity measurements on rare-earth double oxides R2M2O7 Blöte, H. W. J.; Wielinga, R. F.; Huiskamp, W. J. Physica, Vol. 43, Issue 4 https://doi.org/10.1016/0031-8914(69)90187-6	journal	September 1969
Structural and magnetic investigations of single-crystalline neodymium zirconate pyrochlore ${Nd}_{2} {Zr}_{2} O_{7}$ Hatnean, M. Ciomaga; Lees, M. R.; Petrenko, O. A. Physical Review B, Vol. 91, Issue 17 https://doi.org/10.1103/PhysRevB.91.174416	journal	May 2015
Fluctuations and All-In–All-Out Ordering in Dipole-Octupole ${Nd}_{2} {Zr}_{2} O_{7}$ Lhotel, E.; Petit, S.; Guitteny, S. Physical Review Letters, Vol. 115, Issue 19 https://doi.org/10.1103/PhysRevLett.115.197202	journal	November 2015
The Materials Science beamline upgrade at the Swiss Light Source Willmott, P. R.; Meister, D.; Leake, S. J. Journal of Synchrotron Radiation, Vol. 20, Issue 5 https://doi.org/10.1107/S0909049513018475	journal	July 2013
Recent advances in magnetic structure determination by neutron powder diffraction Rodríguez-Carvajal, Juan Physica B: Condensed Matter, Vol. 192, Issue 1-2 https://doi.org/10.1016/0921-4526(93)90108-I	journal	October 1993
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source Abernathy, D. L.; Stone, M. B.; Loguillo, M. J. Review of Scientific Instruments, Vol. 83, Issue 1 https://doi.org/10.1063/1.3680104	journal	January 2012
Low temperature heat capacity of Nd2Zr2O7 pyrochlore Lutique, S.; Javorský, P.; Konings, R. J. M. The Journal of Chemical Thermodynamics, Vol. 35, Issue 6 https://doi.org/10.1016/S0021-9614(03)00040-5	journal	June 2003
First-principles study of structural, elastic, and bonding properties of pyrochlores Pruneda, J. M.; Artacho, Emilio Physical Review B, Vol. 72, Issue 8 https://doi.org/10.1103/PhysRevB.72.085107	journal	August 2005
Oxide pyrochlores — A review Subramanian, M. A.; Aravamudan, G.; Subba Rao, G. V. Progress in Solid State Chemistry, Vol. 15, Issue 2 https://doi.org/10.1016/0079-6786(83)90001-8	journal	January 1983
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/S0567739476001551	journal	September 1976
Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores Sala, G.; Gutmann, M. J.; Prabhakaran, D. Nature Materials, Vol. 13, Issue 5 https://doi.org/10.1038/nmat3924	journal	April 2014
Magnetic anisotropy of the spin-ice compound Dy2Ti2O7 Fukazawa, H.; Melko, R.; Higashinaka, R. Physical Review B, Vol. 65, Issue 5 https://doi.org/10.1103/PhysRevB.65.054410	journal	January 2002
Specific-heat study of the spin-structural change in pyrochlore ${Nd}_{2} {Mo}_{2} O_{7}$ Onose, Y.; Taguchi, Y.; Ito, T. Physical Review B, Vol. 70, Issue 6 https://doi.org/10.1103/PhysRevB.70.060401	journal	August 2004
Bulk magnetization of the heavy rare earth titanate pyrochlores - a series of model frustrated magnets Bramwell, S. T.; Field, M. N.; Harris, M. J. Journal of Physics: Condensed Matter, Vol. 12, Issue 4 https://doi.org/10.1088/0953-8984/12/4/308	journal	December 1999
Investigations of the effect of nonmagnetic Ca substitution for magnetic Dy on spin-freezing in Dy ₂ Ti ₂ O ₇ Anand, V. K.; Tennant, D. A.; Lake, B. Journal of Physics: Condensed Matter, Vol. 27, Issue 43 https://doi.org/10.1088/0953-8984/27/43/436001	journal	October 2015
Crystal-field excitations in ${Nd}_{2}$ ${CuO}_{4}$ , $\Pr_{2}$ ${CuO}_{4}$ , and related n -type superconductors Boothroyd, A. T.; Doyle, S. M.; Paul, D. Mk. Physical Review B, Vol. 45, Issue 17 https://doi.org/10.1103/PhysRevB.45.10075	journal	May 1992
Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7 Rosenkranz, S.; Ramirez, A. P.; Hayashi, A. Journal of Applied Physics, Vol. 87, Issue 9 https://doi.org/10.1063/1.372565	journal	May 2000
Crystal-field states of Pr $^{3 +}$ in the candidate quantum spin ice Pr $_{2}$ Sn $_{2}$ O $_{7}$ Princep, A. J.; Prabhakaran, D.; Boothroyd, A. T. Physical Review B, Vol. 88, Issue 10 https://doi.org/10.1103/PhysRevB.88.104421	journal	September 2013
Quantum fluctuations in spin-ice-like Pr2Zr2O7 Kimura, K.; Nakatsuji, S.; Wen, J-J. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2914	journal	June 2013
Neutron spectroscopic study of crystal field excitations in ${Tb}_{2} {Ti}_{2} O_{7}$ and ${Tb}_{2} {Sn}_{2} O_{7}$ Zhang, J.; Fritsch, K.; Hao, Z. Physical Review B, Vol. 89, Issue 13 https://doi.org/10.1103/PhysRevB.89.134410	journal	April 2014
Crystal field states of ${Tb}^{3 +}$ in the pyrochlore spin liquid ${Tb}_{2} {Ti}_{2} O_{7}$ from neutron spectroscopy Princep, A. J.; Walker, H. C.; Adroja, D. T. Physical Review B, Vol. 91, Issue 22 https://doi.org/10.1103/PhysRevB.91.224430	journal	June 2015
Spectroscopic Properties of Rare Earths Wybourne, Brian G.; Meggers, William F. Physics Today, Vol. 18, Issue 9 https://doi.org/10.1063/1.3047727	journal	September 1965
Introduction to the Theory of Thermal Neutron Scattering Squires, G. L. https://doi.org/10.1017/CBO9781139107808	book	May 2012
Magnetic Monopoles in Spin Ice Castelnovo, C.; Moessner, R.; Sondhi, S. L. Topologica, Vol. 1, Issue 1 https://doi.org/10.3731/topologica.1.012	journal	January 2008
Introduction to the Theory of Thermal Neutron Scattering Bacon, G. E. Physics Bulletin, Vol. 30, Issue 12 https://doi.org/10.1088/0031-9112/30/12/044	journal	December 1979
Emergence of magnetic long-range order in frustrated pyrochlore Nd$_2$Ir$_2$O$_7$ with metal-insulator transition Tomiyasu, K.; Matsuhira, K.; Iwasa, K. arXiv https://doi.org/10.48550/arxiv.1110.6605	text	January 2011
Quantum spin ices and topological phases from dipolar-octupolar doublets on the pyrochlore lattice Huang, Yi-Ping; Chen, Gang; Hermele, Michael arXiv https://doi.org/10.48550/arxiv.1311.1231	text	January 2013
Monopole ordered phases in dipolar and nearest-neighbours Ising pyrochlore: from spin ice to the "all-in--all-out" antiferromagnet Guruciaga, Pamela C.; Grigera, Santiago A.; Borzi, Rodolfo A. arXiv https://doi.org/10.48550/arxiv.1409.5380	text	January 2014
Magnetic Frustration in Lead Pyrochlores Hallas, A. M.; Arevalo-Lopez, A. M.; Sharma, A. Z. arXiv https://doi.org/10.48550/arxiv.1502.00721	text	January 2015
Investigations of the effect of nonmagnetic Ca substitution for magnetic Dy on spin-freezing in Dy2Ti2O7 Anand, V. K.; Tennant, D. A.; Lake, B. arXiv https://doi.org/10.48550/arxiv.1506.03585	text	January 2015
Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets Hertog, Byron C. den; Gingras, Michel J. P. arXiv https://doi.org/10.48550/arxiv.cond-mat/0001369	text	January 2000

Cited By (12)

Special temperatures in frustrated ferromagnets Bovo, L.; Twengström, M.; Petrenko, O. A. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04297-3	journal	May 2018
REZnAl ₁₁ O ₁₉ (RE = Pr, Nd, Sm–Tb): a new family of ideal 2D triangular lattice frustrated magnets Ashtar, M.; Marwat, M. A.; Gao, Y. X. Journal of Materials Chemistry C, Vol. 7, Issue 32 https://doi.org/10.1039/c9tc02643f	journal	January 2019
Exchange interactions in two-state systems: rare earth pyrochlores Curnoe, S. H. Journal of Physics: Condensed Matter, Vol. 30, Issue 23 https://doi.org/10.1088/1361-648x/aac061	journal	May 2018
Tuning the interactions in the spin-ice materials ${Dy}_{2} {Ge}_{2 - x} {Si}_{x} O_{7}$ by silicon substitution Stöter, T.; Antlauf, M.; Opherden, L. Physical Review B, Vol. 100, Issue 5 https://doi.org/10.1103/physrevb.100.054403	journal	August 2019
Monte Carlo study on the detection of classical order by disorder in real antiferromagnetic Ising pyrochlores Guruciaga, Pamela C.; Borzi, Rodolfo A. Physical Review B, Vol. 100, Issue 17 https://doi.org/10.1103/physrevb.100.174404	journal	November 2019
Theory of quantum kagome ice and vison zero modes Huang, Yi-Ping; Hermele, Michael Physical Review B, Vol. 95, Issue 7 https://doi.org/10.1103/physrevb.95.075130	journal	February 2017
Spin clusters and low-energy excitations in rare earth kagome systems Hoch, M. J. R. Modern Physics Letters B, Vol. 31, Issue 01 https://doi.org/10.1142/s0217984916300106	journal	January 2017
Symmetry Enriched U(1) Topological Orders for Dipole-Octupole Doublets on a Pyrochlore Lattice Li, Yao Dong; Chen, Gang arXiv https://doi.org/10.48550/arxiv.1607.02287	text	January 2016
Hidden multipolar orders of dipole-octupole doublets on a triangular lattice Li, Yao-Dong; Wang, Xiaoqun; Chen, Gang arXiv https://doi.org/10.48550/arxiv.1608.07008	text	January 2016
Exchange interactions in two-state systems: rare earth pyrochlores Curnoe, S. H. arXiv https://doi.org/10.48550/arxiv.1803.09683	text	January 2018
Special temperatures in frustrated ferromagnets Bovo, L.; Twengström, M.; Petrenko, O. A. arXiv https://doi.org/10.48550/arxiv.1805.09332	text	January 2018
Intermultiplet transitions and magnetic long-range order in Sm-based pyrochlores Pecanha-Antonio, Viviane; Feng, Erxi; Sun, Xiao arXiv https://doi.org/10.48550/arxiv.1901.00980	text	January 2019

Similar Records

Deviation from the dipole-ice model in the spinel spin-ice candidate

{MgEr}_{2} {Se}_{4}

Journal Article · Fri Apr 26 00:00:00 EDT 2019 · Physical Review B · OSTI ID:1311258

Reig-i-Plessis, D.; Geldern, S. V.; Aczel, Adam A.; +3 more

Dipolar-octupolar Ising antiferromagnetism in

{Sm}_{2} {Ti}_{2} O_{7}

: A moment fragmentation candidate

Journal Article · Wed Sep 05 00:00:00 EDT 2018 · Physical Review B · OSTI ID:1311258

Mauws, Cole; Hallas, A. M.; Sala, Gabriele; +14 more

Dipolar Spin Ice Regime Proximate to an All-In-All-Out Néel Ground State in the Dipolar-Octupolar Pyrochlore

{Ce}_{2} {Sn}_{2} O_{7}

Journal Article · Tue Jan 16 00:00:00 EST 2024 · Physical Review. X · OSTI ID:1311258

Yahne, D. R.; Placke, B.; Schäfer, R.; +11 more

Related Subjects

36 MATERIALS SCIENCE
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS

Title: Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd 2 Zr 2 O 7

Citation Formats

References (49)

Cited By (12)

Similar Records

Related Subjects

Title: Magnetic structure and crystal-field states of the pyrochlore antiferromagnet ${Nd}_{2} {Zr}_{2} O_{7}$