Magnetism of single crystalline breathing pyrochlore spinel AgInCr₄S₈

Single crystals of AgInCr₄S₈ are grown by chemical vapor transport and crystallographic ordering of Ag/In that results in a breathing pyrochlore motif of Cr³⁺ is verified by x-ray and neutron diffraction. Long-range antiferromagnetic order is observed below a Néel temperature of T_N ≈ 9.6 K. The magnetic properties are characterized using ac and dc magnetization, specific heat capacity, and single crystal neutron diffraction measurements. The specific heat data are characterized by a small lambda anomaly near 9.5 K and the estimated magnetic entropy reaches ≈ 13 of the expected value by 3T_N, suggesting significant short-range order in the paramagnetic phase. Single crystal neutron diffraction evidences an incommensurate spin structure with propagation vector k=(0,0,δ) and δ=0.343 at 5 K. The minimal model that accounts for the data consists of ferromagnetic layers of Cr atoms, with magnetic moments lying in the plane of the layers and modulating in the perpendicular direction to form a helical structure propagating along k. This study represents a rare investigation of single crystals within the family of breathing pyrochlore materials.