title: Transferability of Orthogonal and Nonorthogonal Tight-Binding Models for Aluminum Clusters and Nanoparticles.
abstract: Several semiempirical tight-binding models are parametrized and tested for aluminum clusters and nanoparticles using a data set of 808 accurate AlN (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.
authors.affiliation: Department of Chemistry and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455-0431.
authors.forename: Ahren W
authors.initials: AW
authors.lastname: Jasper
authors.affiliation: Department of Chemistry and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455-0431.
authors.forename: Nathan E
authors.initials: NE
authors.lastname: Schultz
authors.affiliation: Department of Chemistry and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455-0431.
authors.forename: Donald G
authors.initials: DG
authors.lastname: Truhlar