First-principles approach with a pseudohybrid density functional for extended Hubbard interactions

Abstract

For massive database-driven materials research, there are increasing demands for both fast and accurate quantum mechanical computational tools. Contemporary density functional theory (DFT) methods can be fast, sacrificing their accuracy, or be precise, consuming a significant amount of resources. Here, to overcome such a problem, we present a DFT method that exploits self-consistent determinations of the on-site and intersite Hubbard interactions (U and V) simultaneously and obtain band gaps of diverse materials in the accuracy of the GW method at a standard DFT computational cost. To achieve the self-consistent evaluation of U and V, we adapt a recently proposed Agapito–Curtarolo–Buongiorno Nardelli pseudohybrid functional for U to implement a density functional of V. This method is found to be appropriate for considering various interactions such as local Coulomb repulsion, covalent hybridization, and their coexistence. We also obtain good agreements between computed and measured band gaps of low-dimensional systems, thus meriting this approach for large-scale as well as high-throughput calculations for various bulk and nanoscale materials with a higher accuracy.