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

Rameshwar L. Kumawat; Chelsea M. Mueller; George C. Schatz

doi:10.1016/j.cplett.2025.141944

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

Rameshwar L. Kumawat, Chelsea M. Mueller, George C. Schatz^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

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.

Original language	English (US)
Article number	141944
Journal	Chemical Physics Letters
Volume	866
DOIs	https://doi.org/10.1016/j.cplett.2025.141944
State	Published - May 2025

Funding

The authors gratefully acknowledge financial support from the Office of Basic Energy Science, Department of Energy , through grant DE-SC0004752 (theory development) and ARO MURI grant W911NF-20-1-0105 (for applications). Computational research was supported in part through the Quest high-performance computing facility at Northwestern University. The authors also thank group members for their helpful discussions.

Keywords

Benchmarking
Density functional theory
Density functional tight binding
Interaction energies
Pt cluster
Pt-Pt SK parameters

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/j.cplett.2025.141944

Cite this

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title = "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 Ptn clusters (n=2−6,8−10). DFTB geometries closely match DFT, with RMSD under 0.15 {\AA}, 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.",

keywords = "Benchmarking, Density functional theory, Density functional tight binding, Interaction energies, Pt cluster, Pt-Pt SK parameters",

author = "Kumawat, {Rameshwar L.} and Mueller, {Chelsea M.} and Schatz, {George C.}",

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doi = "10.1016/j.cplett.2025.141944",

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AU - Kumawat, Rameshwar L.

AU - Mueller, Chelsea M.

AU - Schatz, George C.

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N2 - 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 Ptn 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.

AB - 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 Ptn 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.

KW - Benchmarking

KW - Density functional theory

KW - Density functional tight binding

KW - Interaction energies

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KW - Pt-Pt SK parameters

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

Abstract

Funding

Keywords

ASJC Scopus subject areas

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