Mesoscale Domain Evolution Mechanism during Alternating Current (AC) Poling of Relaxor Ferroelectrics

Abstract

Ferroelectric domain variants that are energetically equivalent are expected to remain preserved during polarization reversal under a symmetry-preserving electric field. However, recent experiments on relaxor-ferroelectric crystals have revealed irreversible elimination of inclined domain walls during AC poling, while the underlying mesoscale mechanism remains unclear. Here, we investigate the domain-wall motion during AC poling of rhombohedral Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_3$--PbTiO$_3$ single crystals containing both 71$^\circ$ and 109$^\circ$ domain walls within a quasi-two-dimensional laminated geometry using phase-field simulations. The simulations reveal that the domain-wall behavior during polarization reversal depends on the spacing ratio between the 71$^\circ$ and 109$^\circ$ domain walls. Closely spaced 71$^\circ$ domain walls undergo irreversible elimination, whereas more widely separated walls are preserved, while the 109$^\circ$ domain walls remain intact. A threshold ratio for domain-wall elimination is identified and found to depend on the mechanical boundary conditions. By tracking the domain-wall trajectories during the switching process, we attribute this behavior to unsynchronized motion of neighboring 71$^\circ$ domain walls arising from long-range elastic interactions when the walls become strongly coupled. This collective motion breaks the symmetry between energetically equivalent domain variants and leads to irreversible domain-wall elimination during polarization reversal. These findings provide mechanistic insight into collective domain-wall evolution during polarization reversal and suggest that proximity-driven symmetry breaking may provide a mesoscale mechanism for domain engineering in ferroelectric materials with high domain-wall densities.