6533b855fe1ef96bd12b0a4c
RESEARCH PRODUCT
Self-Consistent Charge Density-Functional Tight-Binding Parametrization for Pt–Ru Alloys
Ashwin RamasubramaniamPekka KoskinenHongbo Shisubject
platinaAlloy02 engineering and technologyengineering.material010402 general chemistry01 natural sciencesNanoclustersCondensed Matter::Materials ScienceTight bindingalloysPhysics::Atomic and Molecular ClustersCluster (physics)metalliseoksetplatinumPhysical and Theoretical Chemistryta116density functional theoryta114ChemistrytiheysfunktionaaliteoriaCharge densityCharge (physics)021001 nanoscience & nanotechnology0104 chemical sciencesMaxima and minimaClassical mechanicsChemical physicsengineeringnanohiukkasetnanoparticles0210 nano-technologyParametrizationdescription
We present a self-consistent charge density-functional tight-binding (SCC-DFTB) parametrization for PtRu alloys, which is developed by employing a training set of alloy cluster energies and forces obtained from Kohn-Sham density-functional theory (DFT) calculations. Extensive simulations of a testing set of PtRu alloy nanoclusters show that this SCC-DFTB scheme is capable of capturing cluster formation energies with high accuracy relative to DFT calculations. The new SCC-DFTB parametrization is employed within a genetic algorithm to search for global minima of PtRu clusters in the range of 13-81 atoms and the emergence of Ru-core/Pt-shell structures at intermediate alloy compositions, consistent with known results, is systematically demonstrated. Our new SCC-DFTB parametrization enables computationally inexpensive and accurate modeling of Pt-Ru clusters that are among the best-performing catalysts in numerous energy applications.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2017-03-17 | The Journal of Physical Chemistry A |