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    Tetrahedral ferromagnetic correlations and a glassy-freezing anomaly in the breathing pyrochlore magnet AgInCr4S8 with partial A-site disorder

    Yuya Haraguchi1,*, Masahiro Kitamura1, Masaki Gen2, Yusuke Nambu3, Akira Matsuo2, Koichi Kindo2, Masaki Kondo2, Masashi Tokunaga2, and Hiroko Aruga Katori1

    • *Contact author: chiyuya3@go.tuat.ac.jp

    Phys. Rev. B 113, 214437 – Published 15 June, 2026

    DOI: https://doi.org/10.1103/kwkj-78r8

    Abstract

    We investigate the chromium breathing-pyrochlore sulfide AgInCr4S8, a chromium-based thiospinel, by synchrotron x-ray and neutron powder diffraction, dc magnetization, and heat capacity. Diffraction confirms the F4¯3m breathing structure with alternating large and small Cr4 tetrahedra, a large breathing ratio (d′/d=1.106 at 300 K), and substantial Ag/In intermixing on the A sublattice (∼16%). No structural transition or magnetic Bragg peaks are detected down to 1.5 K. An enlarged low-angle difference plot between the 1.5 and 20 K neutron diffraction patterns shows a weak broad diffuselike enhancement, consistent with short-range or frozen correlated moments within the sensitivity of the present data. Susceptibility yields a positive Weiss temperature θW=+92K and a moment enhancement in 30–60 K, while the magnetic entropy released by ∼30K approaches a scale of order R ln 13, together consistent with the development of short-range tetrahedral ferromagnetic correlations and an effective S=6 cluster-moment picture. A broad susceptibility cusp with ZFC–FC bifurcation and a low-temperature specific-heat anomaly near 9 K indicate a phenomenological glassy-freezing anomaly without long-range order. AgInCr4S8 provides a benchmark for the interplay of strong breathing distortion and quenched A-site disorder in chromium breathing pyrochlores.

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