title: Dielectric Genome of van der Waals Heterostructures.
abstract: Vertical stacking of two-dimensional (2D) crystals, such as graphene and hexagonal boron nitride, has recently lead to a new class of materials known as van der Waals heterostructures (vdWHs) with unique and highly tunable electronic properties. Ab initio calculations should in principle provide a powerful tool for modeling and guiding the design of vdWHs, but in their traditional form such calculations are only feasible for commensurable structures with a few layers. Here we show that the dielectric properties of realistic, incommensurable vdWHs comprising hundreds of layers can be efficiently calculated using a multiscale approach where the dielectric functions of the individual layers (the dielectric building blocks) are computed ab initio and coupled together via the long-range Coulomb interaction. We use the method to illustrate the 2D-3D transition of the dielectric function of multilayer MoS2 crystals, the hybridization of quantum plasmons in thick graphene/hBN heterostructures, and to demonstrate the intricate effect of substrate screening on the non-Rydberg exciton series in supported WS2. The dielectric building blocks for a variety of 2D crystals are available in an open database together with the software for solving the coupled electrodynamic equations.
authors.affiliation: †Center for Atomic-scale Materials Design, Department of Physics, and ‡Center for Nanostructured Graphene, Technical University of Denmark, DK-2800 Kgs. Lyngby, Denmark.
authors.forename: Kirsten
authors.initials: K
authors.lastname: Andersen
authors.affiliation: †Center for Atomic-scale Materials Design, Department of Physics, and ‡Center for Nanostructured Graphene, Technical University of Denmark, DK-2800 Kgs. Lyngby, Denmark.
authors.forename: Simone
authors.initials: S
authors.lastname: Latini
authors.affiliation: †Center for Atomic-scale Materials Design, Department of Physics, and ‡Center for Nanostructured Graphene, Technical University of Denmark, DK-2800 Kgs. Lyngby, Denmark.
authors.forename: Kristian S
authors.initials: KS
authors.lastname: Thygesen
keywords: 2D materials; density functional theory; dielectric function; excitons; plasmons; van der Waals heterostructures