Room Temperature Organic Superconductor?

The electron--phonon coupling in fullerene C28 has been calculated from first principles. The value of the associated coupling constant lambda/N(0) is found to be a factor three larger than that associated with C60. Assuming similar values of the density of levels at the Fermi surface N(0) and of the Coulomb pseudopotential for C28-based solids as those associated with alkali-doped fullerides A3C60, one obtains Tc(C28) \approx 8 Tc(C60).Comment: 10 pages, 2 figure

Elimination of unoccupied state summations in it ab initio self-energy calculations for large supercells

We present a new method for the computation of self-energy corrections in large supercells. It eliminates the explicit summation over unoccupied states, and uses an iterative scheme based on an expansion of the Green's function around a set of reference energies. This improves the scaling of the computational time from the fourth to the third power of the number of atoms for both the inverse dielectric matrix and the self-energy, yielding improved efficiency for 8 or more silicon atoms per unit cell

Quasiparticle Electronic structure of Copper in the GW approximation

We show that the results of photoemission and inverse photoemission experiments on bulk copper can be quantitatively described within band-structure theory, with no evidence of effects beyond the single-quasiparticle approximation. The well known discrepancies between the experimental bandstructure and the Kohn-Sham eigenvalues of Density Functional Theory are almost completely corrected by self-energy effects. Exchange-correlation contributions to the self-energy arising from 3s and 3p core levels are shown to be crucial.Comment: 4 pages, 2 figures embedded in the text. 3 footnotes modified and 1 reference added. Small modifications also in the text. Accepted for publication in PR

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.

Vibrational Study of 13C-enriched C60 Crystals

The infrared (IR) spectrum of solid C60 exhibits many weak vibrational modes. Symmetry breaking due to 13C isotopes provides a possible route for optically activating IR-silent vibrational modes. Experimental spectra and a semi-empirical theory on natural abundance and 13C-enriched single crystals of C60 are presented. By comparing the experimental results with the theoretical results, we exclude this isotopic activation mechanism from the explanation for weakly active fundamentals in the spectra.Comment: Accepted for Phys. Rev. B, typeset in REVTEX v3.0 in LaTeX. Postscript file including figures is available at http://insti.physics.sunysb.edu/~mmartin/papers/c13twocol2.ps File with figures will be e-mailed by reques

Ab initio electronic structure, optical, and magneto-optical properties of MnGaAs digital ferromagnetic heterostructures

We report on a theoretical study of the electronic, optical, and magneto-optical properties of digital ferromagnetic heterostructures based on Mn delta-doped GaAs. We consider different structures corresponding to Mn contents within the range 12%-50% and we study how the system changes as a function of the doping concentration. Our first-principles approach includes the spin-orbit interaction in a fully relativistic pseudopotential scheme and the local-field effect in the description of the optical absorption. We show that Mn d-doped GaAs shares many properties with the uniformly doped Ga1-xMnxAs system, i.e., half-metallicity, similar absorption spectra, and moderate Kerr rotation angles in the visible spectral region

Optical absorption spectra of finite systems from a conserving Bethe-Salpeter equation approach

We present a method for computing optical absorption spectra by means of a Bethe-Salpeter equation approach, which is based on a conserving linear response calculation for electron-hole coherences in the presence of an external electromagnetic field. This procedure allows, in principle, for the determination of the electron-hole correlation function self-consistently with the corresponding single-particle Green function. We analyze the general approach for a "one-shot" calculation of the photoabsorption cross section of finite systems, and discuss the importance of scattering and dephasing contributions in this approach. We apply the method to the closed-shell clusters Na_4, Na^+_9 and Na^+_(21), treating one active electron per Na atom.Comment: 9 pages, 3 figure

Electron-phonon interaction in C70

The matrix elements of the deformation potential of C$_{70}$ are calculated by means of a simple, yet accurate solution of the electron-phonon coupling problem in fullerenes, based on a parametrization of the ground state electronic density of the system in terms of $sp^{2+x}$ hybridized orbitals. The value of the calculated dimensionless total electron-phonon coupling constant is $\lambda\approx0.1$, an order of magnitude smaller than in C$_{60}$, consistent with the lack of a superconducting phase transition in C$_{70}$A$_3$ fullerite, and in overall agreement with measurements of the broadening of Raman peaks in C$_{70}$K$_4$. We also calculate the photoemission cross section of C$_{70}^-$, which is found to display less structure than that associated with C$_{60}^-$, in overall agreement with the experimental findings.Comment: To be published in Phys. Rev.

Scanning tunneling microscopy and Raman spectroscopy of polymeric sp-sp2 carbon atomic wires synthesized on the Au(111) surface

Long linear carbon nanostructures based on sp-hybridization can be synthesized by exploiting on-surface synthesis of halogenated precursors evaporated on Au(111), thus opening a way to investigations by surface-science techniques. By means of an experimental approach combining scanning tunneling microscopy and spectroscopy (STM and STS) with ex situ Raman spectroscopy we investigate the structural, electronic and vibrational properties of polymeric sp-sp2 carbon atomic wires composed by sp-carbon chains connected through phenyl groups. Density-functional-theory (DFT) calculations of the structure and the electronic density of states allow us to simulate STM images and to compute Raman spectra. The comparison of experimental data with DFT simulations unveil the properties and the formation stages as a function of the annealing temperature. Atomic-scale structural information from STM complement the Raman sensitivity to the single molecular bond to open the way to detailed understanding of these novel carbon nanostructures

Supercell technique for total-energy calculations of finite charged and polar systems

We study the behavior of total-energy supercell calculations for dipolar molecules and charged clusters. Using a cutoff Coulomb interaction within the framework of a plane-wave basis set formalism, with all other aspects of the method (pseudopotentials, basis set, exchange-correlation functional) unchanged, we are able to assess directly the interaction effects present in the supercell technique. We find that the supercell method gives structures and energies in almost total agreement with the results of calculations for finite systems, even for molecules with large dipole moments. We also show that the performance of finite-grid calculations can be improved by allowing a degree of aliasing in the Hartree energy, and by using a reciprocal space definition of the cutoff Coulomb interaction