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    Possibility of ferro-octupolar order in Ba2CaOsO6 assessed by x-ray magnetic dichroism measurements

    G. Shibata1,*, N. Kawamura2, J. Okamoto3, A. Tanaka4, H. Hayashi5,6,†, K. Yamaura5,6, H. Y. Huang3, A. Singh3,‡, C. T. Chen3 et al.

    D. J. Huang3,7,8, S. V. Streltsov9,§, and A. Fujimori1,3,7,10,∥

    • *Contact author : shibata.goro@jaea.go.jp
    • †Present address: Institute for Solid State Physics, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan.
    • ‡Present address: Department of Physics and Astrophysics, University of Delhi, Delhi 110007, India.
    • §Contact author : streltsov@imp.uran.ru
    • ∥Contact author : fujimori@phys.s.u-tokyo.ac.jp

    Phys. Rev. B 113, 165151 – Published 28 April, 2026

    DOI: https://doi.org/10.1103/mh1b-q11n

    Abstract

    Localized 5d2 electrons in a cubic crystal field possess multipoles such as electric quadrupoles and magnetic octupoles. We studied the cubic double perovskite Ba2CaOsO6 containing the Os6+ (5d2) ions, which exhibits a phase transition to a ‘‘hidden order’’ below T*∼ 50 K, by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at the Os L2,3 edge. The cubic ligand-field splitting between the t2g and eg levels of Os 5d was deduced by XAS to be ∼4eV. Ligand-field multiplet calculation under fictitious strong magnetic fields indicated that the exchange interaction between nearest-neighbor octupoles should be as strong as ∼1.5meV if a ferro-octupolar order is stabilized in the hidden-ordered state, consistent with the exchange interaction of ∼1meV previously predicted theoretically using model and density functional theory calculations. The temperature dependence of the XMCD spectra is consistent with a ∼18meV residual cubic splitting of the lowest Jeff= 2 multiplet state into the non-Kramers Eg doublet ground state and the T2g triplet excited state.

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