Adsorption of H2O, NH3, CO, NO2, and NO on graphene: A first-principles study

Motivated by the recent realization of graphene sensors to detect individual gas molecules, we investigate the adsorption of H2O, NH3, CO, NO2, and NO on a graphene substrate using first-principles calculations. The optimal adsorption position and orientation of these molecules on the graphene surface is determined and the adsorption energies are calculated. Molecular doping, i.e. charge transfer between the molecules and the graphene surface, is discussed in light of the density of states and the molecular orbitals of the adsorbates. The efficiency of doping of the different molecules is determined and the influence of their magnetic moment is discussed.Comment: 6 pages, 6 figure

First principles investigation of the electronic structure of La2MnNiO6: A room-temperature insulating ferromagnet

Using first principles calculations within DFT based on the full potential APW+lo method, we calculated the electronic and magnetic structures for the ferromagnetic and antiferromagnetic states of La2MnNiO6 and analyzed the site projected density of states and electronic band structures. Our calculations show that the ground state of La2MnNiO6 is ferromagnetic insulating with the magnetization in agreement with Hund's first rule and experimental findings.Comment: 10 pages, 3 figure

The mystery of relationship of mechanics and field in the many-body quantum world

We have revealed three fatal errors incurred from a blind transferring of quantum field methods into the quantum mechanics. This had tragic consequences because it produced crippled model Hamiltonians, unfortunately considered sufficient for a description of solids including superconductors. From there, of course, Fr\"ohlich derived wrong effective Hamiltonian, from which incorrect BCS theory arose. 1) Mechanical and field patterns cannot be mixed. Instead of field methods applied to the mechanical Born-Oppenheimer approximation we have entirely to avoid it and construct an independent and standalone field pattern. This leads to a new form of the Bohr's complementarity on the level of composite systems. 2) We have correctly to deal with the center of gravity, which is under the field pattern "materialized" in the form of new quasipartiles - rotons and translons. This leads to a new type of relativity of internal and external degrees of freedom and one-particle way of bypassing degeneracies (gap formation). 3) The possible symmetry cannot be apriori loaded but has to be aposteriori obtained as a solution of field equations, formulated in a general form without translational or any other symmetry. This leads to an utterly revised view of symmetry breaking in non-adiabatic systems, namely Jahn-Teller effect and superconductivity. These two phenomena are synonyms and share a unique symmetry breaking.Comment: 24 pages, 9 sections; remake of abstract, introduction and conclusion; more physics, less philosoph

Robust ab initio calculation of condensed matter: transparent convergence through semicardinal multiresolution analysis

We present the first wavelet-based all-electron density-functional calculations to include gradient corrections and the first in a solid. Direct comparison shows this approach to be unique in providing systematic ``transparent'' convergence, convergence with a priori prediction of errors, to beyond chemical (millihartree) accuracy. The method is ideal for exploration of materials under novel conditions where there is little experience with how traditional methods perform and for the development and use of chemically accurate density functionals, which demand reliable access to such precision.Comment: 4 pages, 3 figures, 4 tables. Submitted to Phys. Rev. Lett. (updated to include GGA

Ab initio phonon dispersion curves and interatomic force constants of barium titanate

The phonon dispersion curves of cubic BaTiO_3 have been computed within a first-principles approach and the results compared to the experimental data. The curves obtained are very similar to those reported for KNbO_3 by Yu and Krakauer [Phys. Rev. Lett. 74, 4067 (1995)]. They reveal that correlated atomic displacements along chains are at the origin of the ferroelectric instability. A simplified model illustrates that spontaneous collective displacements will occur when a dozen of aligned atoms are coupled. The longitudinal interatomic force constant between nearest neighbour Ti and O atoms is relatively weak in comparison to that between Ti atoms in adjacent cells. The small coupling between Ti and O displacements seems however necessary to reproduce a ferroelectric instability.Comment: 12 pages, 4 figure

Variational finite-difference representation of the kinetic energy operator

A potential disadvantage of real-space-grid electronic structure methods is the lack of a variational principle and the concomitant increase of total energy with grid refinement. We show that the origin of this feature is the systematic underestimation of the kinetic energy by the finite difference representation of the Laplacian operator. We present an alternative representation that provides a rigorous upper bound estimate of the true kinetic energy and we illustrate its properties with a harmonic oscillator potential. For a more realistic application, we study the convergence of the total energy of bulk silicon using a real-space-grid density-functional code and employing both the conventional and the alternative representations of the kinetic energy operator.Comment: 3 pages, 3 figures, 1 table. To appear in Phys. Rev. B. Contribution for the 10th anniversary of the eprint serve

Strain-Dependence of Surface Diffusion: Ag on Ag(111) and Pt(111)

Using density-functional theory with the local-density approximation and the generalized gradient approximation we compute the energy barriers for surface diffusion for Ag on Pt(111), Ag on one monolayer of Ag on Pt(111), and Ag on Ag(111). The diffusion barrier for Ag on Ag(111) is found to increase linearly with increasing lattice constant. We also discuss the reconstruction that has been found experimentally when two Ag layers are deposited on Pt(111). Our calculations explain why this strain driven reconstruction occurs only after two Ag layers have been deposited.Comment: 4 pages, 3 figures, Phys. Rev. B 55 (1997), in pres

Theoretical and computational study of high pressure structures in barium

Recent high pressure work has suggested that elemental barium forms a high pressure self-hosting structure (Ba IV) involving two `types' of barium atom. Uniquely among reported elemental structures it cannot be described by a single crystalline lattice, instead involving two interpenetrating incommensurate lattices. In this letter we report pseudopotential calculations demonstrating the stability and the potentially disordered nature of the `guest' structure. Using band structures and nearly-free electron theory we relate the appearance of Ba IV to an instability in the close-packed structure, demonstrate that it has a zero energy vibrational mode, and speculate about the structure's stability in other divalent elements.Comment: 4 pages and 5 figures. To appear in PR

Coupled cluster calculations of ground and excited states of nuclei

The standard and renormalized coupled cluster methods with singles, doubles, and noniterative triples and their generalizations to excited states, based on the equation of motion coupled cluster approach, are applied to the He-4 and O-16 nuclei. A comparison of coupled cluster results with the results of the exact diagonalization of the Hamiltonian in the same model space shows that the quantum chemistry inspired coupled cluster approximations provide an excellent description of ground and excited states of nuclei. The bulk of the correlation effects is obtained at the coupled cluster singles and doubles level. Triples, treated noniteratively, provide the virtually exact description

Soliton effects in dangling-bond wires on Si(001)

Dangling bond wires on Si(001) are prototypical one dimensional wires, which are expected to show polaronic and solitonic effects. We present electronic structure calculations, using the tight binding model, of solitons in dangling-bond wires, and demonstrate that these defects are stable in even-length wires, although approximately 0.1 eV higher in energy than a perfect wire. We also note that in contrast to conjugated polymer systems, there are two types of soliton and that the type of soliton has strong effects on the energetics of the bandgap edges, with formation of intra-gap states between 0.1 eV and 0.2 eV from the band edges. These intra-gap states are localised on the atoms comprising the soliton.Comment: 6 pages, 3 figures, 3 tables, submitted to Phys. Rev.