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We report that small amounts of metal atom non-stoichiometry are possible inthe ZnCr2O4 and MgCr2O4 spinels. The non-stoichiometry, though less than 2%,significantly impacts TN and the nature of the magnetic correlations above TN.The Zn1+xCr2-xO4 spinel is particularly sensitive. While stoichiometric ZnCr2O4displays antiferromagnetic short range correlations in the susceptibility aboveTN, ferromagnetic correlations are observed in non-stoichiometric, hole dopedZn1+xCr2-xO4. The Mg1+xCr2-xO4 spinels are less profoundly affected bynon-stoichiometry, though significant changes are also observed. We contrastthe magnetic properties of Zn1+xCr2-xO4 and Mg1+xCr2-xO4 (x=0, 0.02, 0.04) withthose of materials with the equivalent amounts of isovalent non-magnetic Ga3+substituted on the Cr3+ site to separate the effects of static site disorderand hole doping.

The Sensitivity of the Magnetic Properties of the ZnCr2O4 and MgCr2O4 Spinels to Non-stoichiometry