Bismuth layer-structured ferroelectrics have received significant attention recently due to their fairly high TC and good fatigue endurance which make them important candidates for non-volatile ferroelectric random access memories (Fe-RAMs) as well as for the piezoelectric device applications at high temperatures. Structure of these compounds is generally described as the pseudo-perovskite block (An-1BnO3n+1)2- sandwiched between the bismuth oxide layers (Bi2O2)2+ along the c-axis, where n represents the number of corner sharing BO6 octahedra forming the perovskite-like slabs. Only a few compounds belonging to this family show relaxor behavior (frequency dependent diffuse phase transition). Relaxor ferroelectrics are very attractive for a variety of applications, such as capacitors, sensors, actuators, and integrated electromechanical systems. The present work attempts to understand the mechanism of relaxor behavior in Aurivillius oxides as well as to improve the piezoelectric and ferroelectric properties of some of the known phases. Details pertaining to the fabrication and characterization of BaBi4Ti4O15 (n = 4 member of Aurivillius family of oxides) ceramics are presented. X-ray diffraction, Raman spectroscopy, Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) were employed to probe the structural and microstructural details. The contribution of irreversible domain wall movement to the room temperature dielectric constant and polarization was quantitatively evaluated using the nonlinear dielectric response. Dielectric dispersion and conduction mechanism of these ceramics are also explicated using the complex impedance spectroscopy. The effects of La3+ and Ca2+ doping on the phase transition behavior and other properties of BaBi4Ti4O15 are investigated. La3+ doping for Bi3+ was found to strengthen the relaxor behavior. New compounds such as CaNaBi2Nb3O12, SrNaBi2Nb3O12, Na0.5La0.5Bi4Ti4O12, etc. belonging to the Aurivillius family of oxides have been synthesized and investigations concerning their structural, dielectric and ferroelectric properties are presented. Rietveld refinement of room temperature X-ray powder data suggested that CaNaBi2Nb3O12 and SrNaBi2Nb3O12crystallize in the orthorhombic space group B2cb. SrNaBi2Nb3O12 ceramics exhibited frequency-dependent Tm which follows the Vogel-Fulcher relation implying a relaxor nature. No frequency dependence of Tm was observed for CaNaBi2Nb3O12 ceramics. Polarization - electric field hysteresis loops recorded well above Tm confirmed the coexistence of polar and non-polar domains in SrNaBi2Nb3O12 ceramics. Dielectric anomaly observed around 675 K for CNBN corresponds to the ferroelectric to paraelectric phase transition which is accompanied by the change in crystal structure from orthorhombic to tetragonal. Fe and Nb co-doped Bi4Ti3O12 ceramics were fabricated and characterized for their structural, electrical and magnetic properties.

Relaxor ferroelectrics have been a subject of intense research owing to their interesting physical properties such as high dielectric constant and giant electro-striction. Unlike the conventional lead based relaxors, the relaxors belonging to Aurivillius family of oxides have received much less attention because of the poor understanding of the origin of the relaxor behavior and high processing temperatures involved. In the present investigations, an attempt has been made to understand the origin of relaxor behavior of the materials belonging to Aurivillius family of oxides. The structure and relaxor behavior of BaBi2Nb2O9 (BBN) has been established via the XRD, electron diffraction and dielectric spectroscopy. The results are compared with that of a normal ferroelectric like SrBi2Nb2O9 belonging to the same family as well with that of a conventional relaxor like PMN. The results indicate that the dielectric behavior of BBN is significantly different from that of the conventional relaxors like BBN with very slow broadening of relaxation times and was attributed to the absence of significant polar ordering. To substantiate the existing understanding, studies have been carried out by adopting different strategies such as B-site and A-site cationic substitutions and texturing of the ceramics. Vanadium doping on B-site was found to decrease the sintering temperatures significantly. Aliovalent La3+ doping was found to affect the dielectric behavior strongly with substantial decrease of the freezing temperature and dielectric constants which shows that the relaxor behavior of BBN is highly sensitive to A-site order-disorder. The (00l) textured ceramic of pure and vanadium doped BBN was fabricated via a simple melt-quenching technique and was found to exhibit a significant dielectric and pyroelectric anisotropy. A new class of relaxor compositions (K0.5La0.5Bi2Nb2O9 & K0.5La0.5Bi2Ta2O9) have been synthesized and characterized. These new compounds exhibited interesting physical properties which are akin to that of the conventional lead based relaxors. The presence of superlattice reflections in the electron diffractin patterns recorded on these compounds establish the presence of polar nano regions of significant size. These relaxor crystallites at nano/micro level embedded in a glass matrix have been found to be very promising from their physical properties view point.

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