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We report a comprehensive study on the magnetic and structural properties ofthe spinel sulfides LiInCr4S8, LiGaCr4S8, and CuInCr4S8, where Li+/Cu+ andGa3+/In3+ ions form a zinc-blende-type order. On the basis of synchrotron X-raydiffraction and magnetization data obtained using polycrystalline samples,these three sulfides are suggested to be breathing pyrochlore magnets withalternating antiferromagnetic and ferromagnetic interactions on the small andlarge tetrahedra, respectively. The measured magnetization processes of thethree sulfides up to 72 T are significantly different. The magnetization curvesof LiInCr4S8 and CuInCr4S8 have large hysteresis loops with different shapes,while there is no hysteresis in that of LiGaCr4S8. Geometrical frustration ofthe small tetrahedron is likely to give rise to a wide variety of groundstates, indicating the rich physics in these antiferromagnetic-ferromagneticbreathing pyrochlore magnets.

journal of the physical society of japan

Magnetic and Structural Properties of A-Site Ordered Chromium Spinel  Sulfides: Alternating Antiferromagnetic and Ferromagnetic Interactions in the  Breathing Pyrochlore Lattice