Hybrid Density Functional Tight Binding (DFTB)Molecular Mechanics Approach for a Low-Cost Expansion of DFTB Applicability

• Published in: Journal of chemical theory and computation Vol. 19; no. 15; pp. 5189 - 5198
• Main Authors: Budiutama, Gekko, Li, Ruicheng, Manzhos, Sergei, Ihara, Manabu
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 08.08.2023
• Subjects: Accuracy; Binding; Condensed Matter, Interfaces, and Materials; Density functional theory; Mechanics; Mechanics (physics); Mixed oxides; Modelling; Parameterization; Parameters; Scale (corrosion); Two dimensional materials
• ISSN: 1549-9618; 1549-9626
• DOI: 10.1021/acs.jctc.3c00310

The density functional-based tight binding (DFTB) method has seen a rise in adoption for materials modeling, as it offers significant improvement in scalability with accuracy comparable to the density functional theory (DFT) when good parameterizations exist. The cost reduction in DFTB compared to DFT is achieved by the pre-parameterization of the elements of the Hamiltonian matrix as well as the repulsion potential between all pairs of atoms. Parameterization for new systems with accuracies competitive with DFT in specific applications requires specialized manpower and computational resources. This prevents the application of the DFTB method to systems for which it was not parameterized. In this work, we explore an approach to address the problem of missing parameters of DFTB by modeling the interactions with missing Slater–Koster parameters with an interatomic interaction potential. When the distance between two atoms modeled at the force-field level is sufficiently large, the approach results in accurate structural and electronic properties. The resulting calculation is therefore a hybrid between DFTB and molecular mechanics, a pure DFTB for atoms with a complete set of interatomic parameterizations, and a mix between DFTB and molecular mechanics for atoms with a missing interatomic parameterization. The approach is expected to be particularly useful for hybrid materials and interfaces. The method is tested on the examples of 2D materials, mixed oxides, and a large-scale calculation of an oxide–oxide interface.