Identification of the defect distribution at ferroelectric domain walls from the evolution of nonlinear dielectric response during aging process

TL;DR

This paper develops a thermodynamic model linking microscopic domain wall motion modes to macroscopic dielectric response, enabling analysis of defect distribution changes during ferroelectric aging using simple measurements.

Contribution

It introduces a method to distinguish between different domain wall motion mechanisms and defect distributions during aging through nonlinear dielectric response analysis.

Findings

Reversible domain wall motion can be split into bending and uniform movement modes.

The dominant mode can change with defect distribution during aging.

Macroscopic dielectric measurements can reveal defect arrangements at domain walls.

Abstract

Motion of ferroelectric domain walls greatly contributes to the macroscopic dielectric and piezoelectric response of ferroelectric materials. The domain wall motion through the ferroelectric material is however hindered by pinning on crystal defects which substantially reduces these contributions. Here, using thermodynamic models based on the Landau-Ginzburg-Devonshire theory, we find a relation between microscopic reversible motion of non-ferroelastic 180-degree domain walls interacting with a periodic array of pinning centers and the nonlinear macroscopic permittivity. We show, that the reversible motion of domain walls can be split into two basic modes. First, the bending of a domain wall between pinning centers, and, second, the uniform movement of domain wall plane. We show that their respective contributions may change when the distribution of pinning centers is rearranged during the material aging. We demonstrate that it is possible to indicate which mechanism of the domain wall motion is affected during material aging. This allows to judge whether the defects only homogeneously accumulate at domain walls or prefer to align in certain directions inside the domain wall plane. We suggest that this information can be obtained using simple macroscopic dielectric measurements and a proper analysis of the nonlinear response. Our results may therefore serve as a simple and useful tool to obtain details on domain wall pinning in an aging process.