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Phonons Reflect Dynamic Spin-State Order in LaCoO3

Alsu Ivashko1, Taishun Manjo2,3, Maximilian Kauth1, Yuliia Tymoshenko1, Adrian M. Merritt4, Klaus-Peter Bohnen1, Rolf Heid1, Michael Merz1,5, Andreas Eich1 et al.

John-Paul Castellan1,6, Alexandre Ivanov7, Nathaniel Schreiber8, Hong Zheng8, J. F. Mitchell8, Martin Meven9,10, Jitae T. Park11, Daisuke Ishikawa2,3, Yuiga Nakamura12, Alfred Q. R. Baron2,3, and Frank Weber1

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Phys. Rev. Lett. 137, 116101 – Published 11 September, 2026

DOI: https://doi.org/10.1103/tsw6-sdhk

Abstract

We investigate lattice dynamics in LaCoO3 using inelastic neutron and x-ray scattering over T=2−650  K, spanning the spin-state crossover at T1≈100  K and the insulator-metal transition at T2≈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 T1≤T≤T2 and localized in momentum space at qSSO=(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 La1−xSrxCoO3−λ, J. Phys. Chem. Solids 6, 287 (1958)]. Our results provide momentum-resolved evidence for dynamic correlations of high-spin and low-spin Co3+ states characterized by qSSO=(½,½,½)c, demonstrating that phonons are sensitive probes of fluctuating spin-state correlations in LaCoO3.

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Phys. Rev. Lett. 137, 116101– Published 11 September, 2026
  • Received 23 January 2026
  • Accepted 7 August 2026
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