Abstract
The crystal chemistry and magnetic properties for two triple perovskites, Ba3Fe1.56Ir1.44O9 and Ba3NiIr2O9, grown as large, highly faceted single crystals from a molten strontium carbonate flux, are reported. Unlike the idealized A3MM2'O9 hexagonal symmetry characteristic of most triple perovskites, including Ba3NiIr2O9, Ba3Fe1.56Ir1.44O9 possesses significant site-disorder, resulting in a noncentrosymmetric polar structure with trigonal symmetry. The valence of iron and iridium in the heavily distorted Fe/Ir sites was determined to be Fe(III) and Ir(V) by X-ray absorption near edge spectroscopy (XANES). Density functional theory calculations were conducted to understand the effect of the trigonal distortion on the local Fe(III)O6 electronic structure, and the spin state of iron was determined to be S = 5/2 by Mössbauer spectroscopy. Conductivity measurements indicate thermally activated semiconducting behavior in the trigonal perovskite. Magnetic properties were measured and near room temperature magnetic ordering (TN = 270 K) was observed for Ba3Fe1.56Ir1.44O9.
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