Induction and Ferroelectric Switching of Flux Closure Domains in Strained PbTiO<sub>3</sub> with Neural Network Quantum Molecular Dynamics.

Linker, Thomas M; Nomura, Ken-Ichi; Fukushima, Shogo; Kalia, Rajiv K; Krishnamoorthy, Aravind; Nakano, Aiichiro; Shimamura, Kohei; Shimojo, Fuyuki et al. · Nano Lett · 2023

basic_science · Level V

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Abstract

We have developed an extension of the Neural Network Quantum Molecular Dynamics (NNQMD) simulation method to incorporate electric-field dynamics based on Born effective charge (BEC), called NNQMD-BEC. We first validate NNQMD-BEC for the switching mechanisms of archetypal ferroelectric PbTiO<sub>3</sub> bulk crystal and 180° domain walls (DWs). NNQMD-BEC simulations correctly describe the nucleation-and-growth mechanism during DW switching. In triaxially strained PbTiO<sub>3</sub> with strain conditions commonly seen in many superlattice configurations, we find that flux-closure texture can be induced with application of an electric field perpendicular to the original polarization direction. Upon field reversal, the flux-closure texture switches via a pair of transient vortices as the intermediate state, indicating an energy-efficient switching pathway. Our NNQMD-BEC method provides a theoretical guidance to study electro-mechano effects with existing machine learning force fields using a simple BEC extension, which will be relevant for engineering applications such as field-controlled switching in mechanically strained ferroelectric devices.