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1.
Phys Chem Chem Phys ; 14(43): 14764-8, 2012 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-22532176

RESUMEN

A series of clusters with the general formula CBe(5)E(-) (E = Al, Ga, In, Tl) are theoretically shown to have a planar pentacoordinate carbon atom. The structures show a simple and rigid topological framework-a planar EBe(4) ring surrounding a C center, with one of the ring Be-Be bonds capped in-plane by a fifth Be atom. The system is stabilized by a network of multicenter σ bonds in which the central C atom is the acceptor, and π systems as well by which the C atom donates charge to the Be and E atoms that encircle it.

2.
Chem Commun (Camb) ; 47(22): 6242-4, 2011 Jun 14.
Artículo en Inglés | MEDLINE | ID: mdl-21461423

RESUMEN

We describe and explain the fluxionality of B(13)(+). The chemical bonding analysis shows that the inner triangle of B(13)(+) is bound to the peripheral ring by delocalized bonds only, allowing a quasi-free rotation of the inner ring.

3.
J Am Chem Soc ; 131(26): 9426-31, 2009 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-19507894

RESUMEN

We have explored in detail the potential energy surfaces of the Si(5)Li(n)(5-6) (n = 5-7) systems. We found that it is feasible to design three-dimensional star-like silicon structures using the appropriate ligands. The global minimum structure for Si(5)Li(7)(+) has a perfect seven-peak star-like structure. The title compounds comprise, essentially, the Si(5)(6-) ring interacting with lithium cations. The ionic character of the Si-Li interactions induces the formation of a bridged structure. Concomitantly, our calculations show that the reduction of the Pauli repulsion and the maximization of the orbital contribution are also significant for the star-like structure formation. Additionally, the MO analysis of the systems suggests that the role of the lithium atoms is to provide the precise number of electrons to the central Si(5) unit. This is confirmed by the magnetic properties, which show that electron delocalization enhances the stability of the star-like structures proposed here.

4.
J Chem Phys ; 123(2): 24102, 2005 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-16050736

RESUMEN

We show that the exact non-Born-Oppenheimer Schrodinger equation for the Hookean diatomic molecule H2 (a two-proton, two-electron system where the electron-proton interaction is harmonic while the proton-proton and electron-electron interactions are Coulombic) can be decoupled into equations describing the relative motion of the electrons, the relative motion of nuclei, the motion of a collective mode representing a three-dimensional harmonic oscillator, and the motion of a free particle expressed as a linear combination of the individual center-of-mass coordinates of the nuclei and electrons. Analytic solutions to the relative motion of electrons can be readily obtained for the given values of the harmonic coupling constant. However, exact analytic solutions to the equation for the relative motion of the nuclei cannot be obtained simultaneously due to the fact that the harmonic constants in these two equations are coupled. For this reason, we present for the relative nuclear motion approximate analytic wave functions, one of them obtained variationally and the other by a series solution where the coefficients are determined recursively. We also explore a variational solution to the Taylor-series expansion of the nuclear interaction potential. Properties of the electronic and nuclear intracule densities are examined at different values of the coupling constant. An interesting result of the present non-Born-Oppenheimer treatment of this harmonic model is the fact that the relative nuclear motion occurs in a highly correlated regime. This leads in a natural way to a spatial localization of the nuclei akin to Wigner electronic crystallization.

5.
J Chem Phys ; 120(2): 540-7, 2004 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-15267888

RESUMEN

A reinterpretation of the Boyd-Coulson [R. J. Boyd and C. A. Coulson, J. Phys. B 7, 1805 (1974)] definition of the Fermi hole is presented. Through this reinterpretation, which makes no reference to the hypothetical Hartree level, we are able to show the essentially identical character of the Boyd-Coulson definition with the one based on a conditional probability analysis. The basis-set dependence of the Fermi hole is emphasized and the effect of canonical, localized and delocalized Kohn-Sham and Hartree-Fock basis sets is examined for selected atoms and molecules.

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