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Phonons Reflect Dynamic Spin-State Order in LaCoO 3

Physical Review Letters, vol. 137, pp. 116101

Abstract

We investigate lattice dynamics in LaCoO_{3} using inelastic neutron and x-ray scattering over T=2-650 K, spanning the spin-state crossover at T_{1}≈100 K and the insulator-metal transition at T_{2}≈550 K. Comparison with quasiharmonic ab initio lattice-dynamical calculations helps reveal anomalous softening of a≈10-meV oxygen phonon, confined to the temperature interval T_{1}≤T≤T_{2} and localized in momentum space at q_{SSO}=(½,½,½)_{c}. This wave vector is characteristic of the spin-state-ordering pattern originally proposed by Goodenough [An interpretation of the magnetic properties of the perovskite-type mixed crystals La_{1-x}Sr_{x}CoO_{3-λ}, J. Phys. Chem. Solids 6, 287 (1958)JPCSAW0022-369710.1016/0022-3697(58)90107-0]. Our results provide momentum-resolved evidence for dynamic correlations of high-spin and low-spin Co^{3+} states characterized by q_{SSO}=(½,½,½)_{c}, demonstrating that phonons are sensitive probes of fluctuating spin-state correlations in LaCoO_{3}.

Authors 20

  1. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  2. Affiliation as printed

    Materials Dynamics Laboratory

    Precision Spectroscopy Division

  3. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  4. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  5. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  6. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  7. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  8. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  9. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

  10. Karlsruhe Institute of Technology · Centre National de la Recherche Scientifique · Commissariat à l'Énergie Atomique et aux Énergies Alternatives · CEA Paris-Saclay - Etablissement de Saclay · Laboratoire Léon Brillouin · CEA Paris-Saclay

    Affiliation as printed

    CEA Saclay

    Karlsruhe Institute of Technology

    Laboratoire Léon Brillouin (CEA-CNRS)

  11. Institut Laue-Langevin

    Affiliation as printed

    Institut Laue-Langevin

  12. Argonne National Laboratory

    Affiliation as printed

    Argonne National Laboratory

  13. Argonne National Laboratory

    Affiliation as printed

    Argonne National Laboratory

  14. Argonne National Laboratory

    Affiliation as printed

    Argonne National Laboratory

  15. Martin Meven Aachen

    Forschungszentrum Jülich · Heinz Maier-Leibnitz Zentrum · RWTH Aachen University

    Affiliation as printed

    Forschungszentrum Jülich GmbH at Heinz Maier-Leibnitz Zentrum (MLZ)

    RWTH Aachen University

  16. Heinz Maier-Leibnitz Zentrum

    Affiliation as printed

    Heinz Maier-Leibnitz Zentrum (MLZ)

  17. Affiliation as printed

    Materials Dynamics Laboratory

    Precision Spectroscopy Division

  18. SPring-8 · Japan Synchrotron Radiation Research Institute

    Affiliation as printed

    JASRI

    SPring-8

  19. Affiliation as printed

    Materials Dynamics Laboratory

    Precision Spectroscopy Division

  20. Karlsruhe Institute of Technology

    Affiliation as printed

    Karlsruhe Institute of Technology

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References 66