Niobium oxide dihalides NbOX2: a new family of two-dimensional van der Waals layered materials with intrinsic ferroelectricity and antiferroelectricity
Two-dimensional (2D) ferroelectric (FE) materials displaying the spontaneous polarizations are promising candidates for miniaturized electronic and memory devices. However, stable FE orderings are found in very rare class of 2D materials by experiment so far. In current work, based on high-throughput screening of 2D van der Waals layered materials database and first-principles calculations, we demonstrate niobium oxide dihalides NbOX2 (X = Cl, Br and I), a group of experimentally synthesized yet underexplored van der Waals layered compounds, as a new family of 2D materials that simultaneously exhibit intrinsic in-plane ferroelectricity and antiferroelectricity. Similar to FE perovskite oxides, polar displacement of Nb cations relative to the center of anion octahedral cage can lead to experimentally measurable FE polarizations up to 27 μC/cm2 in layered NbOX2. The presence of low-lying antiferroelectric (AFE) phases can effectively reduce the energy barrier associated with polarization switching, suggesting switchable ferroelectricity is experimentally achievable. In addition, mechanism driving FE phase transitions in NbOX2 monolayer around Curie temperature TC is clearly revealed by our finite-temperature simulations. NbOCl2 monolayer is predicted to be stable ferroelectrics with TC above room temperature. Moreover, application of NbOBr2 and NbOI2 monolayers as 2D dielectric capacitor is further developed, where electrostatic energy storage of nearly 100 % efficiency can be achieved at 2D single-layer regime.