Efficient density functional tight-binding parameterization for accurate modeling of platinum clusters

Abstract

This study presents self-consistent charge DFTB (SCC-DFTB) Slater–Koster parameters for modeling the ground-state properties of Pt nanoclusters. Parameters refined from bulk Pt properties accurately capture potential energy landscapes for Pt${}_n$ clusters ($n=2-6,8-10$). DFTB geometries closely match DFT, with RMSD under 0.15 Å, although DFTB underestimates formation energies due to semi-empirical limitations. Spin-state predictions differ slightly, but singlet-triplet energy separations are negligible (0.05 eV/atom) for $n>4$. Testing on larger clusters ($n=14$–54) showed excellent agreement with DFT, confirming the reliability of these parameters for modeling structural and energetic properties, crucial for catalysis applications.