Obtaining Robust Density Functional Tight-Binding Parameters for Solids across the Periodic Table

Titelangaben

Cui, Mengnan ; Reuter, Karsten ; Margraf, Johannes T.:
Obtaining Robust Density Functional Tight-Binding Parameters for Solids across the Periodic Table.
In: Journal of Chemical Theory and Computation. Bd. 20 (2024) Heft 12 . - S. 5276-5290.
ISSN 1549-9626
DOI: https://doi.org/10.1021/acs.jctc.4c00228

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Abstract

The density functional tight-binding (DFTB) approach allows electronic structure-based simulations at length and time scales far beyond what is possible with first-principles methods. This is achieved by using minimal basis sets and empirical approximations. Unfortunately, the sparse availability of parameters across the periodic table is a significant barrier to the use of DFTB in many cases. We therefore propose a workflow that allows the robust and consistent parametrization of DFTB across the periodic table. Importantly, our approach requires no element-pairwise parameters so that the parameters can be used for all element combinations and are readily extendable. This is achieved by parametrizing all elements on a consistent set of artificial homoelemental crystals, spanning a wide range of coordination environments. The transferability of the resulting periodic table baseline parameters to multielement systems and unknown structures is explored and the model is extensively benchmarked against previous specialized and general DFTB parametrizations.