Epitaxially ferroelectric hexagonal boron nitride on graphene

Abstract Ferroelectricity in two-dimensional (2D) van der Waals (vdW) layers has revolutionized our understanding of the vdW layered coupling, and has been introduced in the domains of moiré superlattice patterns generated by interlayer twisting or sliding. In the smallest limit of thickness, untwisted and epitaxial vdW stacking layers exhibiting ferroelectricity would clearly serve as building blocks for realizing 2D devices with nonvolatile and reconfigurable functionalities. In this study, we grew ferroelectric hexagonal boron nitride (h-BN) films on single-crystal graphene synthesized on a SiC (0001) substrate using nitrogen plasma-assisted molecular beam epitaxy (PA-MBE). Systematic angle-resolved photoemission spectroscopy (ARPES) studies and first-principles calculations revealed that the epitaxial mono-, bi-, and tri-layer h-BN films exhibit layer-number-dependent µ-band dispersions due to an AB stacking sequence on a Bernal-stacked graphene substrate. Furthermore, our piezoelectric force microscopy (PFM) confirmed the coexistence of robust moiré and sliding ferroelectricity at the well-aligned h-BN/graphene heterojunction and in multilayered h-BN films, respectively. In principle, as-developed epitaxially ferroelectric h-BN is limited only by the size of the crystalline graphene substrate, thereby providing a versatile and scalable 2D ferroelectric platform with promising exotic physics and vdW device applications down to a few atomic layers.