2,184 research outputs found
Surface resonance of the (2×1) reconstructed lanthanum hexaboride (001)-cleavage plane : a combined STM and DFT study
We performed a combined study of the (001)-cleavage plane of lanthanum hexaboride (LaB6) using scanning tunneling microscopy and density-functional theory (DFT). Experimentally, we found a (2×1) reconstructed surface on a local scale. The reconstruction is only short-range ordered and tends to order perpendicularly to step edges. At larger distances from surface steps, the reconstruction evolves to a labyrinthlike pattern. These findings are supported by low-energy electron diffraction experiments. Slab calculations within the framework of DFT show that the atomic structure consists of parallel lanthanum chains on top of boron octahedra. Scanning tunneling spectroscopy shows a prominent spectral feature at −0.6eV. Using DFT, we identify this structure as a surface resonance of the (2×1) reconstructed LaB6 (100) surface which is dominated by boron dangling bond states and lanthanum d states
Acceleration Schemes for Ab-Initio Molecular Dynamics and Electronic Structure Calculations
We study the convergence and the stability of fictitious dynamical methods
for electrons. First, we show that a particular damped second-order dynamics
has a much faster rate of convergence to the ground-state than first-order
steepest descent algorithms while retaining their numerical cost per time step.
Our damped dynamics has efficiency comparable to that of conjugate gradient
methods in typical electronic minimization problems. Then, we analyse the
factors that limit the size of the integration time step in approaches based on
plane-wave expansions. The maximum allowed time step is dictated by the highest
frequency components of the fictitious electronic dynamics. These can result
either from the large wavevector components of the kinetic energy or from the
small wavevector components of the Coulomb potential giving rise to the so
called {\it charge sloshing} problem. We show how to eliminate large wavevector
instabilities by adopting a preconditioning scheme that is implemented here for
the first-time in the context of Car-Parrinello ab-initio molecular dynamics
simulations of the ionic motion. We also show how to solve the charge-sloshing
problem when this is present. We substantiate our theoretical analysis with
numerical tests on a number of different silicon and carbon systems having both
insulating and metallic character.Comment: RevTex, 9 figures available upon request, to appear in Phys. Rev.
A fourfold coordinated point defect in silicon
Due to their technological importance, point defects in silicon are among the
best studied physical systems. The experimental examination of point defects
buried in bulk is difficult and evidence for the various defects usually
indirect. Simulations of defects in silicon have been performed at various
levels of sophistication ranging from fast force fields to accurate density
functional calculations. The generally accepted viewpoint from all these
studies is that vacancies and self interstitials are the basic point defects in
silicon. We challenge this point of view by presenting density functional
calculations that show that there is a new fourfold coordinated point defect in
silicon that is lower in energy
All-electron magnetic response with pseudopotentials: NMR chemical shifts
A theory for the ab initio calculation of all-electron NMR chemical shifts in
insulators using pseudopotentials is presented. It is formulated for both
finite and infinitely periodic systems and is based on an extension to the
Projector Augmented Wave approach of Bloechl [P. E. Bloechl, Phys. Rev. B 50,
17953 (1994)] and the method of Mauri et al [F. Mauri, B.G. Pfrommer, and S.G.
Louie, Phys. Rev. Lett. 77, 5300 (1996)]. The theory is successfully validated
for molecules by comparison with a selection of quantum chemical results, and
in periodic systems by comparison with plane-wave all-electron results for
diamond.Comment: 25 pages, 4 tables, submitted to Physical Review
Band-theoretical prediction of magnetic anisotropy in uranium monochalcogenides
Magnetic anisotropy of uranium monochalcogenides, US, USe and UTe, is studied
by means of fully-relativistic spin-polarized band structure calculations
within the local spin-density approximation. It is found that the size of the
magnetic anisotropy is fairly large (about 10 meV/unit formula), which is
comparable with experiment. This strong anisotropy is discussed in view of a
pseudo-gap formation, of which crucial ingredients are the exchange splitting
of U 5f states and their hybridization with chalcogen p states (f-p
hybridization). An anomalous trend in the anisotropy is found in the series
(US>>USe<UTe) and interpreted in terms of competition between localization of
the U 5f states and the f-p hybridization. It is the spin-orbit interaction on
the chalcogen p states that plays an essential role in enlarging the strength
of the f-p hybridization in UTe, leading to an anomalous systematic trend in
the magnetic anisotropy.Comment: 4 pages, 5 figure
First-Principles Electronic Structure of Solid Picene
To explore the electronic structure of the first aromatic superconductor,
potassium-doped solid picene which has been recently discovered by Mitsuhashi
et al with the transition temperatures K, we have obtained a
first-principles electronic structure of solid picene as a first step toward
the elucidation of the mechanism of the superconductivity. The undoped crystal
is found to have four conduction bands, which are characterized in terms of the
maximally localized Wannier orbitals. We have revealed how the band structure
reflects the stacked arrangement of molecular orbitals for both undoped and
doped (Kpicene) cases, where the bands are not rigid. The Fermi surface for
Kpicene is a curious composite of a warped two-dimensional surface and a
three-dimensional one.Comment: 5 pages, 4 figure
An Experimental and Theoretical Study of the Variation of 4f Hybridization Across the La1-xCexIn3 Series
Crystal structures of a series of La1-xCexIn3 (x = 0.02, 0.2, 0.5, or 0.8)
intermetallic compounds have been investigated by both neutron and X-ray
diffraction, and their physical properties have been characterized by magnetic
susceptibility and specific heat measurements. Our results emphasize atypical
atomic displacement parameters (ADP) for the In and the rare-earth sites.
Depending on the x value, the In ADP presents either an "ellipsoidal"
elongation (La-rich compounds) or a "butterfly-like" distortion (Ce-rich
compounds). These deformations have been understood by theoretical techniques
based on the band theory and are the result of hybridization between conduction
electrons and 4f-electrons.Comment: 7 pages, 8 figure
Ab initio investigation of VOSeO3, a spin gap system with coupled spin dimers
Motivated by an early experimental study of VOSeO3, which suggested that it
is a quasi-2D system of weakly coupled spin dimers with a small spin gap, we
have investigated the electronic structure of this material via
density-functional calculations. These ab initio results indicate that the
system is better thought of as an alternating spin-1/2 chain with moderate
interchain interactions, an analog of (VO)2P2O7. The potential interest of this
system for studies in high magnetic field given the presumably small value of
the spin gap is emphasized.Comment: 4 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.
Phase Separation in LiFePO Induced by Correlation Effects
We report on a significant failure of LDA and GGA to reproduce the phase
stability and thermodynamics of mixed-valence LiFePO compounds.
Experimentally, LiFePO compositions () are known to be
unstable and phase separate into Li FePO and FePO. However,
first-principles calculations with LDA/GGA yield energetically favorable
intermediate compounds an d hence no phase separation. This qualitative failure
of LDA/GGA seems to have its origin in the LDA/GGA self-interaction which de
localizes charge over the mixed-valence Fe ions, and is corrected by explicitly
considering correlation effects in this material. This is demonstrated with
LDA+U calculations which correctly predict phase separation in LiFePO
for eV. T he origin of the destabilization of intermediate
compounds is identified as electron localization and charge ordering at
different iron sites. Introduction of correlation also yields more accurate
electrochemical reaction energies between FePO/LiFePO and
Li/Li electrodes.Comment: 12 pages, 5 figures, Phys. Rev. B 201101R, 200
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