Herein, the structure and magnetic properties of the breathing pyrochlore compound LiInCr4−xFexO8 (x = 0, 0.2, 0.4, 0.5) are reported. Raman scattering experiments show the hardening behavior of the active mode induced by the increased ionic masses and bond strength. The long‐range antiferromagnetic order and spin‐gap state of parent samples are found to be suppressed with the increasing Fe content. The average magnetic exchange couplings are strongly antiferromagnetic and systematically enhanced with substitution. Bulk magnetization data of substituted samples show weak ferromagnetic interaction and occurrence of a spin‐glass‐like transition at high Fe contents.
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