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  • Letter
  • Open Access

Spin waves and magnetic Hamiltonian in the low-temperature phase of LiInCr4O8

Gøran J. Nilsen1,2,*, Rafał Wawrzyńczak3,4, Harald O. Jeschke5,†, Hannu Mutka3, Takatsugu Masuda6, Nicola Casati7, Vladimir Pomjakushin8, Zenji Hiroi6, and Yoshihiko Okamoto6

  • *Contact author: goran.nilsen@stfc.ac.uk
  • †Contact author: jeschke@okayama-u.ac.jp
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Phys. Rev. B 112, L020403 – Published 14 July, 2025

DOI: https://doi.org/10.1103/wjh8-qt1x

Abstract

Transition metal spinels, particularly those containing chromium 3+ ions (Cr3+), display a rich variety of low-temperature magnetostructural states. Here, we present a combined neutron scattering, synchrotron x-ray diffraction, and density functional theory study of the frustrated “breathing pyrochlore” chromium spinel LiInCr4O8, where the adjacent Cr3+ tetrahedra alternate in magnetic interaction strength. We first establish the low-temperature tetragonal structure from the diffraction measurements. Considering the magnetic structure in light of the distortions generated by this structure, the short magnetic correlation length found in a previous study can be explained by dimensional reduction due to residual frustration. The Heisenberg Hamiltonian for the low-temperature structure is extracted using density functional theory-based energy mapping and clearly shows the partial release of frustration due to the structural transition. The first four exchanges terms dominate, and the two nearest-neighbor exchanges J and J′ in the high-temperature structure both split substantially. The full magnetic excitation spectrum obtained by inelastic neutron scattering can be accurately reproduced by a linear spin-wave theory model using the density functional exchange parameters as a starting point. However, it is found that multiple parameter sets that obey the relation (J1+J4)/(J2+J3)∼1.24, J1>J2, and J3>J4 provide an equally good description of the data. This ratio, along with the low-temperature structure, suggests that it is the distortion of the small tetrahedra that drives the magnetostructural transition.

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Phys. Rev. B 112, L020403– Published 14 July, 2025
  • Received 6 March 2025
  • Accepted 6 June 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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