Novel Aurivillius Bi4Ti3−2xNbxFexO12 phases with increasing magnetic-cation fraction until percolation: a novel approach for room temperature multiferroism†
Aurivillius oxides with general formula (Bi2O2)(Am−1BmO3m+1) are being extensively investigated for room-temperature multiferroism and magnetoelectric coupling. The chemical design strategy behind current investigations is the incorporation of magnetically active BiMO3 units (M: Fe3+, Mn3+, Co3+…) to the pseudoperovskite layer of known ferroelectrics like Bi4Ti3O12, increasing m. The percolation of magnetic cations at the B-site sublattice is required for magnetic ordering and thus, phases with m ≥ 5 are searched. Alternatively, one can try to directly substitute magnetic species for Ti4+ in the perovskite slab, without introducing additional oxygen octahedra. We report here the mechanosynthesis of Aurivillius Bi4Ti3−2xNbxFexO12 phases with increasing x values up to 1. A maximum magnetic fraction of 1/3, surpassing the threshold for percolation, was reached. Preliminary structural analysis indicated a continuous solid solution, though hints of structural changes between x = 0.25 and 0.5 were found. Ceramic processing was accomplished by spark plasma sintering of the mechanosynthesized phases, including those with high-x ones with reduced thermal stability. This has enabled us to carry out full electrical characterization and to demonstrate ferroelectricity for all phases up to x = 1. Magnetic measurements were also carried out, and weak ferromagnetism was found for x = 1. Therefore, Bi4TiNbFeO12 is proposed to be a novel room-temperature multiferroic.
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