Polycrystalline samples of BaTiO3 doped with 2.0 at. % Mn were prepared by solid-state reaction at various temperatures (Tan) ranging from 500 to 1350 °C, used high-pure powders of BaCO3, TiO2, and MnCO3 as precursors. Experimental results obtained from x-ray diffraction patterns and Raman scattering spectra reveal that tetragonal Mn-doped BaTiO3 starts constituting as Tan ≈ 500 °C. The Tan increase leads to the development of this phase. Interestingly, there is the tetragonal-hexagonal transformation in the crystal structure of BaTiO3 as Tan ≈ 1100 °C. Such the variations influence directly magnetic properties of the samples. Besides paramagnetic contributions of Mn2+ centers traced to electron spin resonance, the room-temperature ferromagnetism found in the samples is assigned to exchange interactions taking place between Mn3+ and Mn4+ ions located in tetragonal BaTiO3 crystals.

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We prepared a polycrystalline sample of orthorhombic La0.7Ca0.3Mn0.85Ni0.15O3, and then studied its critical behavior. Based on the Landau phase-transition theory and Banerjee's criteria, we have found the sample undergoing a second-order magnetic phase transition. This continuous transition is characterized by critical parameters of TC = 170 K, β = 0.320 ± 0.009, γ = 0.990 ± 0.082, and δ = 4.09 ± 0.17 determined from modified Arrott plots. With these values, the magnetization-field-temperature (M-H-T) behaviors of La0.7Ca0.3Mn0.85Ni0.15O3 below and above TC are well described by an equation of state M(H,ε)=εβf±(H/εβ+γ), where ε=(T−TC)/TC, f+ for T > TC and f− for T < TC. Having compared to the theoretical models, the critical-exponent values determined in our case are close to those expected for the 3D Ising model and mean-field theory. This indicates an existence of ferromagnetic short-range interactions in the system below TC. The nature of the transformation from first-order to second-order phase transitions related to the Ni doping is discussed in detail.

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