High-refractive index and mechanically cleavable non-van der Waals InGaS3

Abstract The growing family of two-dimensional crystals has been recognized as a promising platform for investigation of rich low-dimension physics and production of a variety of devices. Of particular interest are recently reported atomic sheets of non-van der Waals materials, which reshape our understanding of chemical bonds and enable heterostructures with novel functionality. Here, we study the structural and optical properties of ultrathin non-van der Waals InGaS 3 sheets produced by standard mechanical cleavage. Our ab initio calculations reveal weak out-of-plane covalent bonds, responsible for the layered structure of the material. The energy required for isolation of a single layer is as low as ~50 meVÅ –2 , which is comparable with the conventional van der Waals material’s monolayer isolation energies of 20–60 meVÅ –2 . A comprehensive study of the structural, vibrational, and optical properties of the material reveals its wide bandgap (2.73 eV), high refractive index (>2.5) and negligible losses in the visible and infrared spectral ranges. These properties make it a perfect candidate for visible-range all-dielectric nanophotonics.