159 research outputs found
A theoretical analysis of the chemical bonding and electronic structure of graphene interacting with Group IA and Group VIIA elements
We propose a new class of materials, which can be viewed as graphene
derivatives involving Group IA or Group VIIA elements, forming what we refer to
as graphXene. We show that in several cases large band gaps can be found to
open up, whereas in other cases a semimetallic behavior is found. Formation
energies indicate that under ambient conditions, sp and mixed sp/sp
systems will form. The results presented allow us to propose that by careful
tuning of the relative concentration of the adsorbed atoms, it should be
possible to tune the band gap of graphXene to take any value between 0 and 6.4
eV.Comment: 5 pages, 4 figures. Transferred to PR
Adsorption of Cu, Ag, and Au atoms on graphene including van der Waals interactions
We performed a systematic density functional study of the adsorption of
copper, silver, and gold adatoms on graphene, especially accounting for van der
Waals interactions by the vdW-DF and the PBE+D2 methods. In particular, we
analyze the preferred adsorption site (among top, bridge, and hollow positions)
together with the corresponding distortion of the graphene sheet and identify
diffusion paths. Both vdW schemes show that the coinage metal atoms do bind to
the graphene sheet and that in some cases the buckling of the graphene can be
significant. The results for silver are at variance with those obtained with
GGA, which gives no binding in this case. However, we observe some quantitative
differences between the vdW-DF and the PBE+D2 methods. For instance the
adsorption energies calculated with the PBE+D2 method are systematically higher
than the ones obtained with vdW-DF. Moreover, the equilibrium distances
computed with PBE+D2 are shorter than those calculated with the vdW-DF method
Accurate electronic band gap of pure and functionalized graphane from GW calculations
Using the GW approximation, we study the electronic structure of the recently
synthesized hydrogenated graphene, named graphane. For both conformations, the
minimum band gap is found to be direct at the point, and it has a
value of 5.4 eV in the stable chair conformation, where H atoms attach C atoms
alternatively on opposite sides of the two dimensional carbon network. In the
meta-stable boat conformation the energy gap is 4.9 eV. Then, using a supercell
approach, the electronic structure of graphane was modified by introducing
either an hydroxyl group or an H vacancy. In this last case, an impurity state
appears at about 2 eV above the valence band maximum.Comment: Submited to Physical Review Letter
Charge self-consistent dynamical mean-field theory based on the full-potential linear muffin-tin orbital method: methodology and applications
Full charge self-consistence (CSC) over the electron density has been
implemented into the local density approximation plus dynamical mean-field
theory (LDA+DMFT) scheme based on a full-potential linear muffin-tin orbital
method (FP-LMTO). Computational details on the construction of the electron
density from the density matrix are provided. The method is tested on the
prototypical charge-transfer insulator NiO using a simple static Hartree-Fock
approximation as impurity solver. The spectral and ground state properties of
bcc Fe are then addressed, by means of the spin-polarized T-matrix fluctuation
exchange solver (SPTF). Finally the permanent magnet SmCo is studied using
multiple impurity solvers, SPTF and Hubbard I, as the strength of the local
Coulomb interaction on the Sm and Co sites are drastically different. The
developed CSC-DMFT method is shown to in general improve on materials
properties like magnetic moments, electronic structure and the materials
density.Comment: 10 pages, 5 figure
Effect of Semicore Orbitals on the Electronic Band Gaps of Si, Ge, and GaAs within the GW Approximation
We study the effect of semicore states on the self-energy corrections and
electronic energy gaps of silicon, germanium and GaAs. Self-energy effects are
computed within the GW approach, and electronic states are expanded in a
plane-wave basis. For these materials, we generate {\it ab initio}
pseudopotentials treating as valence states the outermost two shells of atomic
orbitals, rather than only the outermost valence shell as in traditional
pseudopotential calculations. The resulting direct and indirect energy gaps are
compared with experimental measurements and with previous calculations based on
pseudopotential and ``all-electron'' approaches. Our results show that,
contrary to recent claims, self-energy effects due to semicore states on the
band gaps can be well accounted for in the standard valence-only
pseudopotential formalism.Comment: 6 pages, 3 figures, submitted to Phys. Rev.
Magnetic Lattice Dynamics of the Oxygen-Free FeAs Pnictides: How Sensitive are Phonons to Magnetic Ordering?
To shed light on the role of magnetism on the superconducting mechanism of
the oxygen-free FeAs pnictides, we investigate the effect of magnetic ordering
on phonon dynamics in the low-temperature orthorhombic parent compounds, which
present a spin-density wave. The study covers both the 122 (AFe2As2; A=Ca, Sr,
Ba) and 1111 (AFeAsF; A=Ca, Sr) phases. We extend our recent work on the Ca
(122 and 1111) and Ba (122) cases by treating computationally and
experimentally the 122 and 1111 Sr compounds. The effect of magnetic ordering
is investigated through detailed non-magnetic and magnetic lattice dynamical
calculations. The comparison of the experimental and calculated phonon spectra
shows that the magnetic interactions/ordering have to be included in order to
reproduce well the measured density of states. This highlights a
spin-correlated phonon behavior which is more pronounced than the apparently
weak electron-phonon coupling estimated in these materials. Furthermore, there
is no noticeable difference between phonon spectra of the 122 Ba and Sr,
whereas there are substantial differences when comparing these to CaFe2As2
originating from different aspects of structure and bonding
Modification of activated carbons based on diazonium ions in situ produced from aminobenzene organic acid without addition of other acid
Activated carbon products modified with a benzene sulfonic acid group were prepared based on the spontaneous reduction of diazonium salts in situ generated in water without addition of an external acid. The diazotization reaction assisted by the organic acid substituent, produced at once amine, diazonium and triazene functionalities that maximize the grafting yield by a chemical cooperation effect
Modeling molecular crystals formed by spin-active metal complexes by atom-atom potentials
We apply the atom-atom potentials to molecular crystals of iron (II)
complexes with bulky organic ligands. The crystals under study are formed by
low-spin or high-spin molecules of Fe(phen)(NCS) (phen =
1,10-phenanthroline), Fe(btz)(NCS) (btz = 5,5,6,6-tetrahydro-4\textit{H},4\textit{H}-2,2-bi-1,3-thiazine), and Fe(bpz)(bipy) (bpz =
dihydrobis(1-pyrazolil)borate, and bipy = 2,2-bipyridine). All
molecular geometries are taken from the X-ray experimental data and assumed to
be frozen. The unit cell dimensions and angles, positions of the centers of
masses of molecules, and the orientations of molecules corresponding to the
minimum energy at 1 atm and 1 GPa are calculated. The optimized crystal
structures are in a good agreement with the experimental data. Sources of the
residual discrepancies between the calculated and experimental structures are
discussed. The intermolecular contributions to the enthalpy of the spin
transitions are found to be comparable with its total experimental values. It
demonstrates that the method of atom-atom potentials is very useful for
modeling organometalic crystals undergoing the spin transitions
Possible unconventional superconductivity in iron-based layered compound LaFePO: Study of heat capacity
Heat capacity measurements were performed on recently discovered iron based
layered superconductors, non doped LaFePO and fluorine doped LaFePO. A
relatively large electronic heat capacity coefficient and a small normalized
heat capacity jump at Tc = 3.3 K were observed in LaFePO. LaFePO0.94F0.06 had a
smaller electronic heat capacity coefficient and a larger normalized heat
capacity jump at Tc = 5.8 K. These values indicate that these compounds have
strong electron electron correlation and magnetic spin fluctuation, which are
the signatures of unconventional superconductivity mediated by spin
fluctuation.Comment: 15 Pages, 3 Figure
57Fe Mossbauer spectroscopy and magnetic measurements of oxygen deficient LaFeAsO
We report on the magnetic behavior of oxygen deficient LaFeAsO1-x (x-0.10)
compound, prepared by one-step synthesis, which crystallizes in the tetragonal
(S.G. P4/nmm) structure at room temperature. Resistivity measurements show a
strong anomaly near 150 K, which is ascribed to the spin density wave (SDW)
instability. On the other hand, dc magnetization data shows paramagnetic-like
features down to 5 K, with an effective moment of 0.83 mB/Fe. 57Fe Mossbauer
studies (MS) have been performed at 95 and 200 K. The spectra at both
temperatures are composed of two sub-spectra. At 200 K the major one (88%), is
almost a singlet, and corresponds to those Fe nuclei, which have two oxygen
ions in their close vicinity. The minor one, with a large quadrupole splitting,
corresponds to Fe nuclei, which have vacancies in their immediate neighborhood.
The spectrum at 95 K, exhibits a broadened magnetic split major (84%)
sub-spectrum and a very small magnetic splitting in the minor subspectrum. The
relative intensities of the subspectra facilitate in estimating the actual
amount of oxygen vacancies in the compound to be 7.0(5)%, instead of the
nominal LaFeAsO0.90. These results, when compared with reported 57Fe MS of
non-superconducting LaFeAsO and superconducting LaFeAsO0.9F0.1, confirm that
the studied LaFeAsO0.93 is a superconductivity-magnetism crossover compound of
the newly discovered Fe based superconducting family.Comment: 7 pages text + Figs : Comments/suggestions welcome
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