Construction of optimized tight-binding models using ab initio Hamiltonian: application to monolayer 2H-transition metal dichalcogenides

Abstract

We present optimized tight-binding models with atomic orbitals to improve ab initio tight-binding models constructed by truncating full density functional theory (DFT) Hamiltonian based on localized orbitals. Retaining qualitative features of the original Hamiltonian, the optimization reduces quantitative deviations in overall band structures between the ab initio tight-binding model and the full DFT Hamiltonian. The optimization procedure and related details are demonstrated by using semiconducting and metallic Janus transition metal dichalcogenides monolayers in the 2H configuration. Varying the truncation range from partial second neighbors to third ones, we show differences in electronic structures between the truncated tight-binding model and the original full Hamiltonian, and how much the optimization can remedy the quantitative loss induced by truncation. We further elaborate the optimization process so that local electronic properties such as valence and conduction band edges and Fermi surfaces are precisely reproduced by the optimized tight-binding model. We also extend our discussions to tight-binding models including spin-orbit interactions, so we provide the optimized tight-binding model replicating spin-related properties of the original Hamiltonian such as spin textures. The optimization process described here can be readily applied to construct the fine-tuned tight-binding model based on various DFT calculations.