La3+-induced (micro)structural changes and origin of the relaxor-like phase transition in ferroelectric lead barium niobate electroceramics

Abstract

Lead barium niobate (Pb1-x Ba (x) Nb2O6, PBN) ferroelectric materials have been and are the subject of numerous studies in literature due to their potential for wide-ranging applications in the electronic industry. In this work, La3+-doped Pb0.56Ba0.44Nb2O6 (PBN44) electroceramics were prepared and investigated in terms of X-ray diffraction, scanning electron microscopy, thermal spectra of dielectric permittivity, Curie-Weiss law, and hysteresis loop characteristics. It was noted that La3+ doping favors the formation of orthorhombic mm2 phase in PBN44, which originally shows only the tetragonal 4mm symmetry-related phase. In particular, the PBN44 material with 1 wt% La2O3 displays (micro)structural characteristics and dielectric properties similar to those from PBN compositions lying within their morphotropic phase boundary region. Our results also show that La3+ is able to promote a change of the ferroelectric to paraelectric phase transition appearance of PBN44 from pseudo-normal to really diffuse. However, conversion to a diffuse plus relaxor transition behavior reveals directly linked to incommensurate superstructures present and dielectrically-active in PBN materials toward low temperatures, with an intrinsically frequency-dispersive dielectric response. This statement is also supported by observation of hysteresis loops showing a transformation trend to pseudo-slim-like, even in the normal-like ferroelectrics, when moving into the temperature region of incommensuration manifestation.