Modeling ferroelectric phase transitions with graph convolutional neural networks

Abstract

Ferroelectric materials are widely used in functional devices, however, it has been a long-standing issue to achieve convenient and accurate theoretical modeling of them. Herein, a noval approach to modeling ferroelectric materials is proposed by using graph convolutional neural networks (GCNs). In this approach, the potential energy surface of ferroelectric materials is described by GCNs, which then serves as a calculator to conduct large-scale molecular dynamics simulations. Given atomic positions, the well-trained GCN model can provide accurate predictions of the potential energy and atomic forces, with an accuracy reaching up to 1 meV per atom. The accuracy of GCNs is comparable to that of <i>ab inito</i> calculations, while the computing speed is faster than that of <i>ab inito</i> calculations by a few orders. Benefiting from the high accuracy and fast prediction of the GCN model, we further combine it with molecular dynamics simulations to investigate two representative ferroelectric materials—bulk GeTe and CsSnI₃, and successfully produce their temperature-dependent structural phase transitions, which are in good agreement with the experimental observations. For GeTe, we observe an unusual negative thermal expansion around the region of its ferroelectric phase transition, which has been reported in previous experiments. For CsSnI₃, we correctly obtain the octahedron tilting patterns associated with its phase transition sequence. These results demonstrate the accuracy and reliability of GCNs in the modeling of potential energy surfaces for ferroelectric materials, thus providing a universal approach for investigating them theoretically.