ABSTRACT
Different from conventional 2D sliding ferroelectrics with polarization switchable in the out-of-plane via interlayer sliding, we show the existence of in-plane sliding ferroelectricity in a bilayer of a pentagon-based van der Waals heterostructure formed by vertically stacking an experimentally synthesized penta-PdSe2 sheet and a crystal lattice well-matched penta-PtSe2 sheet. From the 128 sliding patterns, four stable configurations are found that exhibit in-plane sliding ferroelectricity with an ultralow polarization switching barrier of 1.91 meV/atom and a high ferroelectric polarization of ±17.11 × 10-10 C m-1. Following the ferroelectric transition among the stable sliding configurations, significant changes in carrier mobility, electrical conductivity, and second harmonic generation are identified. In particular, the ferroelectric stacking configurations are found to possess a negative Poisson's ratio, facilitating the experimental characterization of the sliding ferroelectric effect. This study demonstrates that pentagonal sheets can be used to realize 2D in-plane sliding ferroelectrics going beyond the existing ones.
ABSTRACT
Pyroelectric materials have been attracting significant attention due to their intrinsic and permanent polarization, where the induced polarization is not associated with specific conditions, such as ferroelectric phase transition, strain gradient, dopants, and electric field. Thus, these materials have great potential for wide applications in energy conversion. Here, we propose a new 3D porous borocarbonitride termed PH-BCN, which is composed of pentagonal motifs with intrinsic polarization along the [0001] direction. Based on first-principles calculations, we show that PH-BCN possesses a record high longitudinal electromechanical coupling coefficient with the value of k33 = 97.99%, a remarkably strong SHG response (χ(2)xzx(0) = χ(2)yzy(0) = χ(2)zxx(0) = χ(2)zyy(0) = -6.23 pm V-1 and χ(2)zzz(0) = 21.21 pm V-1), and a record high shift current value of 908.58 µA V-2 due to the intrinsic vertical polarization. This study expands the family of pentagon-based materials, and may open a new frontier in the design of high-performance pyroelectric materials as well.
