Generation of out-of-plane ferroelectric behavior in a one-atom-thick monolayer

Abstract

Abstract Ferroelectricity with out-of-plane polarization has so far been found in several two-dimensional (2D) materials, including monolayers comprising three to five planes of atoms, e.g. α-In2Se3 and MoTe2. Here, we explore the generation of out-of-plane polarization within a one-atom-thick monolayer material, namely hexagonal boron nitride. We performed density-functional-theory calculations to explore inducing ferroelectric-like distortions through incorporation of isovalent substitutional impurities that are larger than the host atoms. This disparity in bond lengths causes a buckling of the h-BN, either up or down, which amounts to a dipole with two equivalent energies and opposing orientations. We tested several impurities to explore the magnitude of the induced dipole and the switching energy barrier for dipole inversion. The effects of strain, dipole–dipole interactions, and vertical heterostructures with graphene are further explored. Our results suggest a highly-tunable system with ground state antiferroelectricity and metastable ferroelectricity. We expect that this work will help foster new ways to include functionality in layered 2D-material-based applications.