Defect-driven polarization reconfiguration in Bi3.15Nd0.85Ti3O12 film

Abstract

The physical origin of controlling ferroelectric properties in defect-engineered Aurivillius-phase layered materials lies in the local polarization evolution mediated by structural defects. Nevertheless, the role of widely prevalent out-of-phase boundary (OPB) defects in configuring polarization remains unclear. This study uses Bi_3.15Nd_0.85Ti₃O₁₂ film, optimized with a HfO₂ buffer layer, as a model system to elucidate the intrinsic mechanism behind the enhanced local polarization within the OPB defect regions. Atomic-scale quantitative analysis reveals that OPB defects enhance the in-plane displacement of B-site cations and co-align their out-of-plane polarization directions within the perovskite layers. This reconfiguration disrupts the intrinsic antipolar ordering by eliminating the antiparallel alignment of out-of-plane dipoles between adjacent pseudo-perovskite blocks in the pristine lattice. Strain and vacancy redistribution further promote the polarization configuration transition by disrupting charge compensation. These findings provide mechanistic insights into defect-modulated ferroelectricity and suggest a new approach for designing high-performance devices through strain and defect engineering.