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

Abstract

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 TN≈0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) μB/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65μB/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.

Authors:
 [1];  [2];  [3];  [4];  [5];  [4];  [2];  [1]
+ Show Author Affiliations
  1. Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany); Technische Univ. Berlin (Germany)
  2. Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany)
  3. Helmholtz-Zentrum Berlin for Materials and Energy GmbH, Berlin (Germany); Bhabha Atomic Research Centre (BARC), Mumbai (India)
  4. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Helmholtz Virtual Institute
OSTI Identifier:
1311258
Alternate Identifier(s):
OSTI ID: 1234009
Grant/Contract Number:  
AC05-00OR22725; VHVI-521
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 22; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Xu, J., Anand, V. K., Bera, A. K., Frontzek, Matthias D., Abernathy, Douglas L., Casati, N., Siemensmeyer, K., and Lake, B. Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd2Zr2O7. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.224430.
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Xu, J., Anand, V. K., Bera, A. K., Frontzek, Matthias D., Abernathy, Douglas L., Casati, N., Siemensmeyer, K., & Lake, B. Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd2Zr2O7. United States. https://doi.org/10.1103/PhysRevB.92.224430
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Xu, J., Anand, V. K., Bera, A. K., Frontzek, Matthias D., Abernathy, Douglas L., Casati, N., Siemensmeyer, K., and Lake, B. Mon . "Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd2Zr2O7". United States. https://doi.org/10.1103/PhysRevB.92.224430. https://www.osti.gov/servlets/purl/1311258.
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@article{osti_1311258,
title = {Magnetic structure and crystal-field states of the pyrochlore antiferromagnet Nd2Zr2O7},
author = {Xu, J. and Anand, V. K. and Bera, A. K. and Frontzek, Matthias D. and Abernathy, Douglas L. and Casati, N. and Siemensmeyer, K. and Lake, B.},
abstractNote = {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 TN≈0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) μB/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65μB/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.},
doi = {10.1103/PhysRevB.92.224430},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 22,
volume = 92,
place = {United States},
year = {Mon Dec 28 00:00:00 EST 2015},
month = {Mon Dec 28 00:00:00 EST 2015}
}
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https://doi.org/10.1103/PhysRevB.92.224430
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    Works referencing / citing this record:

    Special temperatures in frustrated ferromagnets
    journal, May 2018

    REZnAl 11 O 19 (RE = Pr, Nd, Sm–Tb): a new family of ideal 2D triangular lattice frustrated magnets
    journal, January 2019

    • Ashtar, M.; Marwat, M. A.; Gao, Y. X.
    • Journal of Materials Chemistry C, Vol. 7, Issue 32
    • DOI: 10.1039/c9tc02643f

    Exchange interactions in two-state systems: rare earth pyrochlores
    journal, May 2018

    Tuning the interactions in the spin-ice materials Dy 2 Ge 2 − x Si x O 7 by silicon substitution
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    Hidden multipolar orders of dipole-octupole doublets on a triangular lattice
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    Special temperatures in frustrated ferromagnets
    text, January 2018

    Intermultiplet transitions and magnetic long-range order in Sm-based pyrochlores
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