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Local and average structures of the spin-glass pyrochlore Y2Mo2O7 from neutron diffraction and neutron pair distribution function analysis

J. E. Greedan, Delphine Gout, A. D. Lozano-Gorrin, Shahab Derahkshan, Th. Proffen, H.-J. Kim, E. Božin, and S. J. L. Billinge
Phys. Rev. B 79, 014427 – Published 21 January 2009

Abstract

The observation of canonical spin-glass behavior in the pyrochlore oxide Y2Mo2O7 has been a subject of considerable interest as the original structural studies were interpreted in terms of a well-ordered crystallographic model. It is widely held that the stabilization of the spin-glass state requires some level of positional disorder along with frustration. Recent reports from local probe measurements, extended x-ray-absorption fine structure (EXAFS) and Y89 NMR, have been interpreted in terms of disorder involving the Mo-Mo distances (EXAFS) and multiple Y sites (NMR). This work reports results from temperature-dependent (15–300 K) neutron diffraction (ND) and neutron pair distribution function studies which can provide from the same data set information on both the average and local structures. The principal findings are that: (1) there is no crystallographic phase transition over the temperature region studied within the resolution of the ND data; (2) the diffraction data are well fitted using a fully ordered model but with large and anisotropic displacement parameters for three of the four atomic sites; (3) the pairwise real-space correlation function G(r) shows clear evidence that the principal source of disorder is associated with the Y-O1 atom pairs rather than the Mo-Mo pairs, in disagreement with the interpretation of the EXAFS results; (4) fits to the G(r) improve significantly when anisotropic displacements for all sites are included; (5) inclusion of a split-site position parameter for O1 improves, slightly, both the G(r) fits and the Rietveld fits to the ND data; and (6) for all models the fits become worse as the temperature decreases and as the fitting range decreases. These results are qualitatively consistent with the Y89 NMR observations and perhaps recent muon-spin-relaxation studies. The issue of static versus dynamic disorder is not resolved, definitively. An estimate of the distribution of exchange constants due to the disorder is made using spin-dimer analysis and compared with the Saunders-Chalker model for the generation of spin-glass behavior from “weak” disorder on geometrically frustrated lattices.

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  • Received 18 November 2008

DOI:https://doi.org/10.1103/PhysRevB.79.014427

©2009 American Physical Society

Authors & Affiliations

J. E. Greedan1, Delphine Gout2, A. D. Lozano-Gorrin1, Shahab Derahkshan1, Th. Proffen3, H.-J. Kim3, E. Božin4, and S. J. L. Billinge4

  • 1Department of Chemistry and Brockhouse Institute for Materials Research, McMaster University, Hamilton, Canada L8S 4M1
  • 2Jülich Center for Neutron Science–SNS, Forschungszentrum Jülich, 52425 Jülich, Germany and Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, Tennessee 38371, USA
  • 3Lujan Neutron Scattering Center, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
  • 4Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, USA and Condensed Matter and Materials Science Department, Brookhaven National Laboratory, Upton, New York 11973, USA

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Vol. 79, Iss. 1 — 1 January 2009

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