Self-Consistent Charge Density-Functional Tight-Binding Parametrization for Pt–Ru Alloys

Self-Consistent Charge Density-Functional Tight-Binding Parametrization for Pt–Ru Alloys

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 testin...

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Veröffentlicht in:The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2017-03, Vol.121 (12), p.2497-2502
Hauptverfasser: Shi, Hongbo, Koskinen, Pekka, Ramasubramaniam, Ashwin
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container_title The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory
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creator Shi, Hongbo
Koskinen, Pekka
Ramasubramaniam, Ashwin
description 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.
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title Self-Consistent Charge Density-Functional Tight-Binding Parametrization for Pt–Ru Alloys
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