Breathing pyrochlore lattice realized in A-site ordered spinel oxides LiGaCr4O8 and LiInCr4O8

Abstract

A unique type of frustrated lattice is found in two A-site ordered spinel oxides, LiGaCr4O8 and LiInCr4O8. Because of the large size mismatch between Li+ and Ga3 +/In3+ ions at the A site, the pyrochlore lattice, made up of Cr3+ ions carrying spin 3/2, becomes an alternating array of small and large tetrahedra, i.e., a "breathing" pyrochlore lattice. We introduce a parameter, the breathing factor Bf, which quantifies the degree of frustration in the pyrochlore lattice: Bf is defined as J′/J, where J′ and J are nearest-neighbor magnetic interactions in the large and small tetrahedra, respectively. LiGaCr4O8 with Bf∼0.6 shows magnetic susceptibility similar to that of conventional Cr spinel oxides such as ZnCr2O4. In contrast, LiInCr4O8 with a small Bf∼0.1 exhibits a spin-gap behavior in its magnetic susceptibility, suggesting a proximity to an exotic singlet ground state. Magnetic long-range order occurs at 13.8 and 15.9 K for LiGaCr4O 8 and LiInCr4O8, respectively, in both cases likely owing to the coupling to structural distortions. © 2013 American Physical Society.