Screened-Exchange Range-Separated Hybrid Functionals for Surfaces and Interfaces

Electronic structure calculations based on density functional theory have successfully predicted numerous ground-state properties of a variety of molecules and materials. However, exchange and correlation functionals currently used in the literature, including semi-local and hybrid functionals, are often inaccurate to describe the electronic properties of heterogeneous solids, especially systems composed of building blocks with large dielectric mismatch. Here, we present a dielectric-dependent range separated hybrid functional, screened-exchange range-separated hybrid (SE-RSH) [1], for the investigation of heterogeneous materials. We define a spatially dependent fraction of exact exchange inspired by the static Coulomb-hole and screened-exchange (COHSEX) approximation used in many-body perturbation theory, and we show that the proposed functional accurately predicts the electronic structure of several nonmetallic interfaces, three- and two-dimensional, pristine, and defective solids and nanoparticles.

[1] J. Zhan, M. Govoni, and G. Galli, J. Chem. Theory Comput. (2023)