Thickness-Dependent Evolutions of Surface Reconstruction and Band Structures in Epitaxial -In₂Se₃ Thin Films

Ferroelectric materials have received great attention in the field of data storage, benefiting from their exotic transport properties. Among these materials, the two-dimensional (2D) In2Se3 has been of particular interest because of its ability to exhibit both in-plane and out-of-plane ferroelectricity. In this article, we realized the molecular beam epitaxial (MBE) growth of beta-In2Se3 films on bilayer graphene (BLG) substrates with precisely controlled thickness. Combining in situ scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) measurements, we found that the four-monolayer beta-In2Se3 is a semiconductor with a (9 x 1) reconstructed superlattice. In contrast, the monolayer beta-In2Se3/BLG heterostructure does not show any surface reconstruction due to the interfacial interaction and moire superlattice, which instead results in a folding Dirac cone at the center of the Brillouin zone. In addition, we found that the band gap of In2Se3 film decreases after potassium doping on its surface, and the valence band maximum also shifts in momentum after surface potassium doping. The successful growth of high-quality beta-In2Se3 thin films would be a new platform for studying the 2D ferroelectric heterostructures and devices. The experimental results on the surface reconstruction and band structures also provide important information on the quantum confinement and interfacial effects in the epitaxial beta-In2Se3 films.