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    Excitation spectrum and low-temperature magnetism in the disordered defect-fluorite Ho2Zr2O7

    P. L. Oliveira Silva1,*, J. G. A. Ramon1,2, Viviane Peçanha-Antonio3,4,†, Tatiana Guidi3,5, J. S. Gardner6, Chun Sheng Fang7, and R. S. Freitas1,‡

    • *Contact author: pedrolucas@usp.br
    • †Contact author: viviane.antonio@stfc.ac.uk
    • ‡Contact author: freitas@if.usp.br

    Phys. Rev. B 113, 214423 – Published 8 June, 2026

    DOI: https://doi.org/10.1103/rf1x-8swz

    Abstract

    In this work, we report on the thermomagnetic characterization and crystalline-electric field (CEF) energy scheme of the disordered defect-fluorite Ho2Zr2O7. This structural phase is distinguished by the coexistence of magnetic frustration and extensive disorder, with Ho3+ and Zr4+ sharing randomly the same 4a site with even 50% occupancy, and an average 1/8 oxygen vacancy per unit cell. AC magnetic susceptibility measurements performed on powder samples down to 0.5 K revealed signs of slowing spin dynamics without glassy behavior, including a frequency dependent peak at ∼1K. Yet, no evidence for long-range magnetic order is found down to 200 mK in the specific heat. Inelastic neutron scattering measurements show a weak, low-lying CEF excitation around 2 meV, accompanied by a broad level centered at 60 meV. To fit our observations, we propose an approach to account for structural disorder in the crystal-field splitting of the non-Kramers Ho3+. Our model provides an explanation to the broadening of the high-energy, single-ion excitations and suggests that the zirconate ground-state wavefunction has zero magnetic moment. Through the breaking of local symmetry, structural disorder enables the magnetic response observed in Ho2Zr2O7, allowing the mixing of low-lying states at finite temperatures. Finally, we show that this scenario is in good agreement with the bulk properties reported in this work.

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