Pressure-Induced Simultaneous Metal-Insulator and Structural-Phase Transitions in LiH: a Quasiparticle Study

A pressure-induced simultaneous metal-insulator transition (MIT) and structural-phase transformation in lithium hydride with about 1% volume collapse has been predicted by means of the local density approximation (LDA) in conjunction with an all-electron GW approximation method. The LDA wrongly predicts that the MIT occurs before the structural phase transition. As a byproduct, it is shown that only the use of the generalized-gradient approximation together with the zero-point vibration produces an equilibrium lattice parameter, bulk modulus, and an equation of state that are in excellent agreement with experimental results.Comment: 7 pages, 4 figures, submitted to Europhysics Letter

Density functional investigations of defect induced mid-gap states in graphane

We have carried out ab initio electronic structure calculations on graphane (hydrogenated graphene) with single and double vacancy defects. Our analysis of the density of states reveal that such vacancies induce the mid gap states and modify the band gap. The induced states are due to the unpaired electrons on carbon atoms. Interestingly the placement and the number of such states is found to be sensitive to the distance between the vacancies. Furthermore we also found that in most of the cases the vacancies induce a local magnetic moment.Comment: 15 page

Assessing the Performance of Recent Density Functionals for Bulk Solids

We assess the performance of recent density functionals for the exchange-correlation energy of a nonmolecular solid, by applying accurate calculations with the GAUSSIAN, BAND, and VASP codes to a test set of 24 solid metals and non-metals. The functionals tested are the modified Perdew-Burke-Ernzerhof generalized gradient approximation (PBEsol GGA), the second-order GGA (SOGGA), and the Armiento-Mattsson 2005 (AM05) GGA. For completeness, we also test more-standard functionals: the local density approximation, the original PBE GGA, and the Tao-Perdew-Staroverov-Scuseria (TPSS) meta-GGA. We find that the recent density functionals for solids reach a high accuracy for bulk properties (lattice constant and bulk modulus). For the cohesive energy, PBE is better than PBEsol overall, as expected, but PBEsol is actually better for the alkali metals and alkali halides. For fair comparison of calculated and experimental results, we consider the zero-point phonon and finite-temperature effects ignored by many workers. We show how Gaussian basis sets and inaccurate experimental reference data may affect the rating of the quality of the functionals. The results show that PBEsol and AM05 perform somewhat differently from each other for alkali metal, alkaline earth metal and alkali halide crystals (where the maximum value of the reduced density gradient is about 2), but perform very similarly for most of the other solids (where it is often about 1). Our explanation for this is consistent with the importance of exchange-correlation nonlocality in regions of core-valence overlap.Comment: 32 pages, single pdf fil

Optical signature of symmetry variations and spin-valley coupling in atomically thin tungsten dichalcogenides

Motivated by the triumph and limitation of graphene for electronic applications, atomically thin layers of group VI transition metal dichalcogenides are attracting extensive interest as a class of graphene-like semiconductors with a desired band-gap in the visible frequency range. The monolayers feature a valence band spin splitting with opposite sign in the two valleys located at corners of 1st Brillouin zone. This spin-valley coupling, particularly pronounced in tungsten dichalcogenides, can benefit potential spintronics and valleytronics with the important consequences of spin-valley interplay and the suppression of spin and valley relaxations. Here we report the first optical studies of WS2 and WSe2 monolayers and multilayers. The efficiency of second harmonic generation shows a dramatic even-odd oscillation with the number of layers, consistent with the presence (absence) of inversion symmetry in even-layer (odd-layer). Photoluminescence (PL) measurements show the crossover from an indirect band gap semiconductor at mutilayers to a direct-gap one at monolayers. The PL spectra and first-principle calculations consistently reveal a spin-valley coupling of 0.4 eV which suppresses interlayer hopping and manifests as a thickness independent splitting pattern at valence band edge near K points. This giant spin-valley coupling, together with the valley dependent physical properties, may lead to rich possibilities for manipulating spin and valley degrees of freedom in these atomically thin 2D materials

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

Systematic Study on Fluorine-doping Dependence of Superconducting and Normal State Properties in LaFePO1-xFx

We have investigated the fluorine-doping dependence of lattice constants, transports and specific heat for polycrystalline LaFePO1-xFx. F doping slightly and monotonically decreases the in-plane lattice parameter. In the normal state, electrical resistivity at low temperature is proportional to the square of temperature and the electronic specific heat coefficient has large value, indicating the existence of moderate electron-electron correlation in this system. Hall coefficient has large magnitude, and shows large temperature dependence, indicating the low carrier density and multiple carriers in this system. Temperature dependence of the upper critical field suggests that the system is a two gap superconductor. The F-doping dependence of these properties in this system are very weak, while in the FeAs system (LaFeAsO), the F doping induces the large changes in electronic properties. This difference is probably due to the different F-doping dependence of the lattice in these two systems. It has been revealed that a pure effect of electron doping on electronic properties is very weak in this Fe pnictide compound.Comment: 8 pages, 5 figures, accepted for publication in J. Phys. Soc. Jp

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.

Electronic properties of LaOFFeAs in the normal state probed by NMR/NQR

We report 139La, 57Fe and 75As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements on powders of the new LaO1-xFxFeAs superconductor for x = 0 and x = 0.1 at temperatures up to 480 K, and compare our measured NQR spectra with local density approximation (LDA) calculations. For all three nuclei in the x = 0.1 material, it is found that the local Knight shift increases monotonically with an increase in temperature, and scales with the macroscopic susceptibility, suggesting a single magnetic degree of freedom. Surprisingly, the spin lattice relaxation rates for all nuclei also scale with one another, despite the fact that the form factors for each site sample different regions of q-space. This result suggests a lack of any q-space structure in the dynamical spin susceptibility that might be expected in the presence of antiferromagnetic correlations. Rather, our results are more compatible with simple quasi-particle scattering. Furthermore, we find that the increase in the electric field gradient at the As cannot be accounted for by LDA calculations, suggesting that structural changes, in particular the position of the As in the unit cell, dominate the NQR response.Comment: 17 pages, 6 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 ([email protected]

Self-consistent Spectral Function for Non-Degenerate Coulomb Systems and Analytic Scaling Behaviour

Novel results for the self-consistent single-particle spectral function and self-energy are presented for non-degenerate one-component Coulomb systems at various densities and temperatures. The GW^0-method for the dynamical self-energy is used to include many-particle correlations beyond the quasi-particle approximation. The self-energy is analysed over a broad range of densities and temperatures (n=10^17/cm^3-10^27/cm^3, T=10^2 eV/k_B-10^4 eV/k_B). The spectral function shows a systematic behaviour, which is determined by collective plasma modes at small wavenumbers and converges towards a quasi-particle resonance at higher wavenumbers. In the low density limit, the numerical results comply with an analytic scaling law that is presented for the first time. It predicts a power-law behaviour of the imaginary part of the self-energy, Im Sigma ~ -n^(1/4). This resolves a long time problem of the quasi-particle approximation which yields a finite self-energy at vanishing density.Comment: 28 pages, 9 figure