Transferability of Orthogonal and Nonorthogonal Tight-Binding Models for Aluminum Clusters and Nanoparticles

Several semiempirical tight-binding models are parametrized and tested for aluminum clusters and nanoparticles using a data set of 808 accurate Al N (N = 2−177) energies and geometries. The effects of including overlap when solving the secular equation and of incorporating many-body (i.e., nonpairwi...

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Bibliographic Details
Published in:Journal of chemical theory and computation 2007-01, Vol.3 (1), p.210-218
Main Authors: Jasper, Ahren W, Schultz, Nathan E, Truhlar, Donald G
Format: Article
Language:English
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Summary:Several semiempirical tight-binding models are parametrized and tested for aluminum clusters and nanoparticles using a data set of 808 accurate Al N (N = 2−177) energies and geometries. The effects of including overlap when solving the secular equation and of incorporating many-body (i.e., nonpairwise) terms in the repulsion and electronic matrix elements are studied. Pairwise orthogonal tight-binding (TB) models are found to be more accurate and their parametrizations more transferable (for particles of different sizes) than both pairwise and many-body nonorthogonal tight-binding models. Many-body terms do not significantly improve the accuracy or transferability of orthogonal TB, whereas some improvement in the nonorthogonal models is observed when many-body terms are included in the electronic Hamiltonian matrix elements.
ISSN:1549-9618
1549-9626
DOI:10.1021/ct600261s