Two-dimensional ferroelectricity induced by octahedral rotation distortion in perovskite oxides

Abstract

Two-dimensional (2D) ferroelectricity has attracted extensive attention since its discovery in the monolayers of van der Waals materials. Here we show that 2D ferroelectricity induced by octahedral rotation distortion is widely present in the perovskite bilayer system through first-principles calculations. Perovskite tolerance factor plays a crucial role in the lattice dynamics and groundstate structure of the perovskite monolayers and bilayers, thus providing an important indicator for screening this hybrid improper ferroelectricity. Generally, the ferroelectric switching via an orthorhombic twin state has the lowest energy barrier. Epitaxial strain can effectively tune the ferroelectric polarization and ferroelectric switching by changing the amplitude of octahedral rotation and tilt distortion. The increasing compressive strain causes a polar to non-polar phase transition by suppressing the tilt distortion. The cooperative effect of octahedral distortion at the interface with the substrate can reduce the energy barrier of reversing rotation mode, and even change the lowest-energy ferroelectric switching path.