Piezoelectric and other physical properties are significantly enhanced at (or near) a morphotropic phase boundary (MPB) in ferroelectrics. MPB materials have attracted significant attention owing to both fundamental physics as well as the possibility of wellregulated energy and information storage devices which are dominated by lead (Pb)-based materials. Here, we report the crystal structure, Raman spectra, dielectric constant and polarization near the MPB of lead free (1 − x) Na 0.5 Bi 0.5 TiO 3 − x BaTiO 3 (0.00 ⩽ x ⩽ 0.10) solid-solution, prepared by sol-gel auto combustion technique and sintered by microwave sintering technique. With the addition of BaTiO 3 into Na 0.5 Bi 0.5 TiO 3 , it induces a structural phase transition from R3c (a single phase) to R3c + P4mm (a dual phase) close to x = 0.06 and 0.07 and transform to a high symmetry tetragonal phase P4mm at higher compositions (x = 0.08 to 0.10) as evident from our x-ray Rietveld refinement and Raman spectroscopic results. We perform first-principles calculations based on density functional theory that confirm a structural transition from a rhombohedral to a tetragonal phase under increasing x. In the prepared solid solution, an anomalous enhancement of remnant polarization (2P 0 r ) was observed for x = 0.06 and 0.07, which has been explained based on the existence of the MPB. On the other hand, the value of coercive field E 0 C was found to be decreased linearly from x = 0.00 to 0.06; it is constant for higher compositions. Further details of the ferroelectric properties on the electric field poled samples have been studied and compared with the as-grown (unpoled) samples.
Multiferroic composites are promising candidates for magnetic field sensors, next-generation low power memory and spintronic devices, as they exhibit much higher magnetoelectric (ME) coupling and coupled ordering parameters compared to the single-phase multiferroics. Hence, the 3-0 type particulate multiferroic composites having general formula (1 − Φ)[PbFe0.5Nb0.5O3]-Φ[Co0.6Zn0.4Fe1.7Mn0.3O4] (Φ = 0.0, 0.05, 0.1, 0.2, 0.3, 0.4, 0.5, 1.0, (1 − Φ) PFN-ΦCZFMO) were prepared using a hybrid synthesis technique. Preliminary structural and microstructural analysis were carried out using XRD and FESEM techniques, which suggest the formation of 3-0 type particulate composite without the presence of any impurity phases. The multiferroic behaviour of the composites is studied with polarization versus electric field (P-E) and magnetization versus magnetic field (M-H) characteristics at room temperature. The nature of ME coupling was investigated elaborately by employing the Landau free energy equation along with the magneto-capacitance measurement. This investigation suggests the existence of biquadratic nature of ME coupling (P2M2). The magneto-electric coupling measurement also suggests that strain mediated domain coupling between the ferroelectric and magnetic ordering is responsible for the magneto-electric behaviour. The obtained value of direct ME coefficient 26.78 mV/cm-Oe for Φ = 0.3, found to be higher than the well-known single-phase materials and polycrystalline composites.
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