Phase-field insight into the nature of topological polarization structures in uniaxial ferroelectrics

Abstract

Uniaxial ferroelectrics have long served as benchmark systems for time-resolved studies of polarization evolution due to their simple 180-domain structure. However, recent experiments in these materials have revealed complex topological textures with enigmatic features, including the unexpected charge-free head-to-head and tail-to-tail domain walls which still wait for their consistent explanation. Here, we use a universal three-dimensional phase-field model to investigate the kinetics of domain structure development in triglycine sulfate, accounting for the monoclinic symmetry of its parent and ferroelectric phases. We show that isolated saddle-like polarization structures, interconnected saddle cascades, saddle lines and specific monkey saddles can form only when transverse degrees of freedom for spontaneous polarization are allowed in the polar plane of a uniaxial ferroelectric. The abundance and diversity of saddle-like structures at the early stages of domain ordering drives a far more effective compensation of bound charges at head-to-head and tail-to-tail domain walls than those predicted by single-component order parameter models. As domains coarsen and residual bound charges migrate toward the surfaces of the sample, the topological landscape simplifies, leaving behind only isolated saddle points. The present model successfully reproduces exotic structures observed experimentally in triglycine sulfate and lead germanate and reveals a domain topology that extends beyond the conventional Ising picture of uniaxial ferroelectrics. Although the mechanisms of bound-charge compensation are likely to be material-specific, similar topological structures may emerge in other uniaxial ferroelectrics. The general formulation of our phase-field model opens the way for future studies of such phenomena across a broader class of ferroelectric materials of arbitrary symmetry.