Atomically thin indium selenide (InSe) is a representative two-dimensional (2D) family that have recently attracted extensive interest for their intriguing emerging physics and potential optoelectronic applications with high-performance. Here, by utilizing molecular beam epitaxy and scanning tunneling microscopy, we report a controlled synthesis of InSe thin films down to the monolayer limit and characterization of their electronic properties at atomic scale. Highly versatile growth conditions are developed to fabricate well crystalline InSe films, with a reversible and controllable phase transformation between InSe and In2Se3. The band gap size of InSe films, as enhanced by quantum confinement, increases with decreasing film thickness. Near various categories of lattice imperfections, the band gap becomes significantly enlarged, resulting in a type-I band alignments for lateral heterojunctions. Such band gap enhancement, as unveiled from our first-principles calculations, is ascribed to the local compressive strain imposed by the lattice imperfections. Moreover, InSe films host highly conductive 2D electron gas, manifesting prominent quasiparticle scattering signatures. The 2D electron gas is self-formed via substrate doping of electrons, which shift the Fermi level above the confinement-quantized conduction band. Our study identifies InSe ultrathin film as an appealing system for both fundamental research and potential applications in nanoelectrics and optoelectronics.
Keywords: InSe films; band bending; density functional theory calculations; molecular beam epitaxy growth; scanning tunneling microscopy; strain effect; two-dimensional electron gas.