Tetrahedral ferromagnetic correlations and a glassy-freezing anomaly in the breathing pyrochlore magnet with partial -site disorder
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 , a chromium-based thiospinel, by synchrotron x-ray and neutron powder diffraction, dc magnetization, and heat capacity. Diffraction confirms the breathing structure with alternating large and small tetrahedra, a large breathing ratio ( at 300 K), and substantial Ag/In intermixing on the sublattice (). 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 and a moment enhancement in 30–60 K, while the magnetic entropy released by approaches a scale of order ln 13, together consistent with the development of short-range tetrahedral ferromagnetic correlations and an effective 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. provides a benchmark for the interplay of strong breathing distortion and quenched -site disorder in chromium breathing pyrochlores.