DFT-based parameterization of a non-orthogonal tight-binding model for electronic band structure calculations of carbon and hydrocarbon materials

The tight-binding model provides a useful alternative to first-principles methods for quantum mechanical modeling of atomic structures and the physicochemical properties of materials. It is well-suited for investigating topologically complex systems with large numbers of atoms, since it substantially reduces the computational cost. However, the accuracy of the tight-binding model critically depends on the choice of parameters. In this work, we introduce a parameterized, non-orthogonal tight-binding model to calculate the electronic properties of carbon and hydrocarbon materials. We performed the parameterization using initial DFT calculations of the electronic band structures of seven carbon and hydrocarbon materials with different dimensionalities and atomic hybridizations. The calculated electronic band structures show reasonable agreement with DFT results. The proposed parameter set is transforable and suitable for different hydrocarbon crystals. As a result, the represented approach can support extensive searches for new materials of this type, as well as more efficient and accurate studies of the electronic band structures of their synthesized counterparts. Furthermore, such synthesis of methods allows the analytical advantages of tight-binding method to be retained while complementing them with the accuracy of ab initio calculations. Thus, this work should contribute to significant improvements in the key performance characteristics of computational materials science methodologies and algorithms.

1. The Ministry of Science and Higher Education of the Russian Federation - Project FSWU-2024-0014