Origin and Reduction of Coercive Fields in ZnO-based Wurtzite Ferroelectrics

Abstract

Wurtzite ferroelectrics offer a route to semiconductor-compatible non-volatile devices, but their large coercive fields (E$_c$) constrain the operating window between polarization reversal, leakage and dielectric breakdown. Atomically localized and non-classical switching fronts have recently been identified in wurtzite nitrides, yet the microscopic feature that sets the coercive field remains unresolved. Here we use large-scale reactive molecular dynamics, parameterized against first-principles data, to follow field-driven reversal in pristine, Mg-modified and heterostructured ZnO. Reversal proceeds through rugged inversion-boundary filaments in agreement with recent observations in other wurtzite ferroelectrics. We find that the field required for switching is controlled by the advancing filament head, which is a under-coordinated reconstructed inversion-boundary region during the transient switching dynamics with a large field-aligned local polar-order amplitude that is only partially compensated by an oppositely oriented surrounding shell. Controlled strain-only and charge-doping-only perturbations show that charge redistribution lowers the coercive field more effectively than strain because it suppresses this field-setting unscreened local polar order at the filament head, with the combined effect lowering E$_c$ by $\sim$ 50 \%. Layered ZnO/ZnMgO architectures further create buried nucleation sites and shorten filament propagation lengths. These results connect atomistic switching topology to a materials-design principle for substantially reducing coercive fields in ZnO-based wurtzite ferroelectrics.