Atomic reconfiguration among tri-state transition at ferroelectric/antiferroelectric phase boundaries in Pb(Zr,Ti)O3

Abstract

Phase boundary provides a fertile ground for exploring emergent phenomena and understanding order parameters couplings in condensed-matter physics. In Pb(Zr1-xTix)O3, there are two types of composition-dependent phase boundary with both technological and scientific importance, i.e. morphotropic phase boundary (MPB) separating polar regimes into different symmetry and ferroelectric/antiferroelectric (FE/AFE) phase boundary dividing polar and antipolar dipole configurations. In contrast with extensive studies on MPB, FE/AFE phase boundary is far less explored. Here, we apply atomic-scale imaging and Rietveld refinement to directly demonstrate the intermediate phase at FE/AFE phase boundary exhibits a rare multipolar Pb-cations ordering, i.e. coexistence of antipolar or polar displacement, which manifests itself in both periodically gradient lattice spacing and anomalous initial hysteresis loop. In-situ electron/neutron diffraction reveals that the same parent intermediate phase can transform into either FE or AFE state depending on suppression of antipolar or polar displacement, coupling with the evolution of long-/short-range oxygen octahedra tilts. First-principle calculations further show that the transition between AFE and FE phase can occur in a low-energy pathway via the intermediate phase. These findings enrich the structural understanding of FE/AFE phase boundary in perovskite oxides.

Giant and reversible photoluminescence modulation based on in situ electric-field-controlled antiferroelectric–ferroelectric phase transition

“…Recently, Fu et al reported an intermediate phase at the AFE/FE phase boundary of PZT, where antipolar and polar displacements of Pb-cations coexist. 46 This intermediate phase serves as a polar ordering “bridge” connecting the AFE and FE phases, similar to the monoclinic phases between the tetragonal and R phases at the morphotropic phase boundary (MPB). 47 Based on our observations, this intermediate phase exists when the applied E is smaller than E AF or E FA .…”

Synergistically Optimizing Pressure-Driven Energy Conversion and Energy-Harvesting Application via Modulating an Antiferroelectric-to-Ferroelectric Overlap Zone in Antiferroelectric Ceramics

“…The main reflections {h00} and {hh0} in x = 0 sample display splitting and the superlattice diffraction peaks occurs around 1/2(110) p , supporting the average structure of the orthorhombic AFE state. 40 It is well-known that the origin of the 1/4(hkl) superlattice diffraction peaks is the antiparallel displacement of the A-site cation and the neighboring apex O 2− ions along the baxis, resulting in the antiferroelectric properties of PbZrO 3 and PLZT materials. 41,42 In the locally magnified diffraction peaks in the range of 36°∼ 45°, with the increasing BAN content, the specific peaks of (111) p are slightly split, and (200) p are gradually merged as well as the superlattice diffraction peaks around 1/2(110) p is weakened by degrees.…”

Enhanced high‐power performance of Fe‐doped PZMNZT piezoelectric ceramics

“…Considerable academic efforts have been made to improve the above parameters, such as structural heterogeneity, 8 designing textured ferroelectric ceramics, [9][10] constructing morphotropic phase boundary (MPB), [11][12] induced isolated-oxygen-vacancy, 13 etc. However, so far, element doping is still a simple and effective method that makes Pb(Zr,Ti)O 3 (PZT)-based ceramics more applicable to high-power applications.…”