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Benchmarking Density Functional Based Tight-Binding for Silver and Gold Materials: From Small Clusters to Bulk

Luiz Oliveira 1 Nathalie Tarrat 2 Jérôme Cuny 3 Joseph Morillo 4 Didier Lemoine 1 Fernand Spiegelman 3 Mathias Rapacioli 3
1 Théorie (LCAR)
LCAR - Laboratoire Collisions Agrégats Réactivité
2 CEMES-SINanO - Surfaces, Interfaces et Nano-Objets
CEMES - Centre d'élaboration de matériaux et d'études structurales
3 MAD - Modélisation, Agrégats, Dynamique (LCPQ)
LCPQ - Laboratoire de Chimie et Physique Quantiques
Abstract : We benchmark existing and improved self-consistent-charge density functional based tight-binding (SCC-DFTB) parameters for silver and gold clusters as well as for bulk materials. In the former case, our benchmarks focus on both the structural and energetic properties of small-size AgN and AuN clusters (N from 2 to 13), medium-size clusters with N = 20 and 55, and finally larger nanoparticles with N = 147, 309, and 561. For bulk materials, structural, energetics and elastic properties are discussed. We show that SCC-DFTB is quite satisfactory in reproducing essential differences between silver and gold aggregates, in particular their 2D–3D structural transitions, and their dependency upon cluster charge. SCC-DFTB is also in agreement with DFT and experiments in the medium-size regime regarding the energetic ordering of the different low-energy isomers and allows for an overall satisfactory treatment of bulk properties. A consistent convergence between the cohesive energies of the largest investigated nanoparticles and the bulk’s is obtained. On the basis of our results for nanoparticles of increasing size, a two-parameter analytical extrapolation of the cohesive energy is proposed. This formula takes into account the reduction of the cohesive energy for undercoordinated surface sites and converges properly to the bulk cohesive energy. Values for the surface sites cohesive energies are also proposed.
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https://hal.archives-ouvertes.fr/hal-01392312
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Submitted on : Friday, November 4, 2016 - 11:39:07 AM
Last modification on : Tuesday, April 5, 2022 - 3:43:33 AM

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Luiz Oliveira, Nathalie Tarrat, Jérôme Cuny, Joseph Morillo, Didier Lemoine, et al.. Benchmarking Density Functional Based Tight-Binding for Silver and Gold Materials: From Small Clusters to Bulk. Journal of Physical Chemistry A, American Chemical Society, 2016, 120 (42), pp.8469-8483. ⟨10.1021/acs.jpca.6b09292⟩. ⟨hal-01392312⟩

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