A Multipolar Approach to Sliding Ferroelectricity

Abstract

Traditional theoretical treatments of ferroelectricity do not straightforwardly extend to sliding ferroelectrics, which are increasingly-studied layered materials where a switchable electrical polarization is controlled by two-dimensional relative motion of the stacked layers. Therefore, in-depth analyses of the underlying processes which dictate their polarization behavior remain challenging. In this paper, we present a comprehensive approach for identifying the symmetry-adapted microscopic parameters which are responsible for driving the emergence of this polarization. First, we outline our approach, which appeals to group theory arguments and the distortion of Wannier orbital densities to connect macroscopic symmetries to the microscopic electronic distortions which dictate the appearance of ferroelectricity. Then, we illustrate this process by using density functional theory to apply our strategy to honeycomb bilayer systems, including hexagonal boron nitride. In this way, we find that combinations of dipole-like and quadrupole-like distortions of lone pair electron orbitals control electronic reorganization, and by extension, ferroelectricity in such systems.