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Observation of Antiferromagnetism in Marokite CaMn2O4

Abstract Marokite (CaMn 2 O 4 ) has been identified as a low-level impurity in the solid-state synthesis of Ca 1− x La x MnO 3 perovskites in the low- x region. In order to properly isolate the complex magnetic behavior of these important perovskites, the low- temperature magnetic structure and properties of marokite are determined and reported. All Mn ions are in the high-spin 3+ oxidation state. Jahn–Teller-distorted MnO 6 octahedra share both edges and vertices in a three-dimensional network, through which various exchange mechanisms cooperatively give rise to antiferromagnetic Mn 3+ spin order. The magnetic order is evidenced below T N =220 K by a peak in the magnetic susceptibility and the appearance of symmetry-lowering magnetic Bragg reflections in neutron diffraction.