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Real-space determination of orbital states driving successive phase transitions in FeV2O4

Chihaya Koyama1,*, Yusuke Nomura2,3, Shunsuke Kitou1,†, Taishun Manjo4, Yuiga Nakamura4, Takeshi Hara5, Naoyuki Katayama6, Yoichi Nii7, Ryotaro Arita8,9 et al.

Hiroshi Sawa10 and Taka-hisa Arima1,9

  • *Contact author: koyama-chihaya@g.ecc.u-tokyo.ac.jp
  • †Contact author: kitou@edu.k.u-tokyo.ac.jp
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Phys. Rev. Research 8, 043058 – Published 16 October, 2026

DOI: https://doi.org/10.1103/j864-1gpm

Abstract

Direct experimental access to orbital states in strongly correlated materials remains a major challenge, despite their central role in driving coupled structural and magnetic phase transitions. In systems where electronic correlations, electron-lattice coupling, and relativistic spin-orbit interactions compete on comparable energy scales, first-principles calculations often yield multiple metastable solutions, hindering the unambiguous identification of the ground state. Here, we demonstrate that the orbital states of the spinel oxide FeV2O4, which possesses active orbital degrees of freedom on both Fe and V ions, are uniquely resolved by combining valence electron density (VED) analysis based on state-of-the-art synchrotron x-ray diffraction with spin-polarized density-functional-theory calculations. Our results reveal that temperature-dependent rearrangements of orbital occupations drive successive structural transitions that accompany collinear and noncoplanar ferrimagnetic ordering, establishing a direct correspondence between orbital anisotropy and spin structure. This work shows that experimentally determined VED provides a decisive real-space constraint on competing theoretical solutions, offering a powerful and broadly applicable framework for elucidating the microscopic mechanisms of complex phase transitions in strongly correlated electron systems.

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Phys. Rev. Research 8, 043058– Published 16 October, 2026
  • Received 9 April 2026
  • Accepted 19 September 2026
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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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