Elementary structural building blocks encountered in silicon surface reconstructions

Driven by the reduction of dangling bonds and the minimization of surface stress, reconstruction of silicon surfaces leads to a striking diversity of outcomes. Despite this variety even very elaborate structures are generally comprised of a small number of structural building blocks. We here identify important elementary building blocks and discuss their integration into the structural models as well as their impact on the electronic structure of the surface

A new structural model for the Si(331)-(12x1) reconstruction

A new structural model for the Si(331)-(12x1) reconstruction is proposed. Based on scanning tunneling microscopy images of unprecedented resolution, low-energy electron diffraction data, and first-principles total-energy calculations, we demonstrate that the reconstructed Si(331) surface shares the same elementary building blocks as the Si(110)-(16x2) surface, establishing the pentamer as a universal building block for complex silicon surface reconstructions

Ab initio study of reflectance anisotropy spectra of a sub-monolayer oxidized Si(100) surface

The effects of oxygen adsorption on the reflectance anisotropy spectrum (RAS) of reconstructed Si(100):O surfaces at sub-monolayer coverage (first stages of oxidation) have been studied by an ab initio DFT-LDA scheme within a plane-wave, norm-conserving pseudopotential approach. Dangling bonds and the main features of the characteristic RAS of the clean Si(100) surface are mostly preserved after oxidation of 50% of the surface dimers, with some visible changes: a small red shift of the first peak, and the appearance of a distinct spectral structure at about 1.5 eV. The electronic transitions involved in the latter have been analyzed through state-by-state and layer-by-layer decompositions of the RAS. We suggest that new interplay between present theoretical results and reflectance anisotropy spectroscopy experiments could lead to further clarification of structural and kinetic details of the Si(100) oxidation process in the sub-monolayer range.Comment: 21 pages, 8 figures. To be published in Physical Rev.

Many-body-QED perturbation theory: Connection to the Bethe-Salpeter equation

The connection between many-body theory (MBPT)--in perturbative and non-perturbative form--and quantum-electrodynamics (QED) is reviewed for systems of two fermions in an external field. The treatment is mainly based upon the recently developed covariant-evolution-operator method for QED calculations [Lindgren et al. Phys. Rep. 389, 161 (2004)], which has a structure quite akin to that of many-body perturbation theory. At the same time this procedure is closely connected to the S-matrix and the Green's-function formalisms and can therefore serve as a bridge between various approaches. It is demonstrated that the MBPT-QED scheme, when carried to all orders, leads to a Schroedinger-like equation, equivalent to the Bethe-Salpeter (BS) equation. A Bloch equation in commutator form that can be used for an "extended" or quasi-degenerate model space is derived. It has the same relation to the BS equation as has the standard Bloch equation to the ordinary Schroedinger equation and can be used to generate a perturbation expansion compatible with the BS equation also for a quasi-degenerate model space.Comment: Submitted to Canadian J of Physic

Exciton-plasmon states in nanoscale materials: breakdown of the Tamm-Dancoff approximation

Within the Tamm-Dancoff approximation ab initio approaches describe excitons as packets of electron-hole pairs propagating only forward in time. However, we show that in nanoscale materials excitons and plasmons hybridize, creating exciton--plasmon states where the electron-hole pairs oscillate back and forth in time. Then, as exemplified by the trans-azobenzene molecule and carbon nanotubes, the Tamm-Dancoff approximation yields errors as large as the accuracy claimed in ab initio calculations. Instead, we propose a general and efficient approach that avoids the Tamm--Dancoff approximation, and correctly describes excitons, plasmons and exciton-plasmon states

Correct quantum chemistry in a minimal basis from effective Hamiltonians

We describe how to create ab-initio effective Hamiltonians that qualitatively describe correct chemistry even when used with a minimal basis. The Hamiltonians are obtained by folding correlation down from a large parent basis into a small, or minimal, target basis, using the machinery of canonical transformations. We demonstrate the quality of these effective Hamiltonians to correctly capture a wide range of excited states in water, nitrogen, and ethylene, and to describe ground and excited state bond-breaking in nitrogen and the chromium dimer, all in small or minimal basis sets

Study of a Nonlocal Density scheme for electronic--structure calculations

An exchange-correlation energy functional beyond the local density approximation, based on the exchange-correlation kernel of the homogeneous electron gas and originally introduced by Kohn and Sham, is considered for electronic structure calculations of semiconductors and atoms. Calculations are carried out for diamond, silicon, silicon carbide and gallium arsenide. The lattice constants and gaps show a small improvement with respect to the LDA results. However, the corresponding corrections to the total energy of the isolated atoms are not large enough to yield a substantial improvement for the cohesive energy of solids, which remains hence overestimated as in the LDA.Comment: 4 postscript figure