123 research outputs found
Stability of Ge-related point defects and complexes in Ge-doped SiO_2
We analyze Ge-related defects in Ge-doped SiO_2 using first-principles
density functional techniques. Ge is incorporated at the level of ~ 1 mol % and
above. The growth conditions of Ge:SiO_2 naturally set up oxygen deficiency,
with vacancy concentration increasing by a factor 10^5 over undoped SiO_2, and
O vacancies binding strongly to Ge impurities. All the centers considered
exhibit potentially EPR-active states, candidates for the identification of the
Ge(n) centers. Substitutional Ge produces an apparent gap shrinking via its
extrinsic levels.Comment: RevTeX 4 pages, 2 ps figure
Neutral-ionic phase transition : a thorough ab-initio study of TTF-CA
The prototype compound for the neutral-ionic phase transition, namely TTF-CA,
is theoretically investigated by first-principles density functional theory
calculations. The study is based on three neutron diffraction structures
collected at 40, 90 and 300 K (Le Cointe et al., Phys. Rev. B 51, 3374 (1995)).
By means of a topological analysis of the total charge densities, we provide a
very precise picture of intra and inter-chain interactions. Moreover, our
calculations reveal that the thermal lattice contraction reduces the indirect
band gap of this organic semi-conductor in the neutral phase, and nearly closes
it in the vicinity of the transition temperature. A possible mechanism of the
neutral-ionic phase transition is discussed. The charge transfer from TTF to CA
is also derived by using three different technics.Comment: 11 pages, 9 figures, 7 table
Ab-initio simulations on growth and interface properties of epitaxial oxides on silicon
The replacement of SiO2 by so-called high-k oxides is one of the major
challenges for the semiconductor industry to date. Based on electronic
structure calculations and ab-initio molecular dynamics simulations, we are
able to provide a consistent picture of the growth process of a class of
epitaxial oxides around SrO and SrTiO3. The detailed understanding of the
interfacial binding principles has also allowed us to propose a way to engineer
the band-offsets between the oxide and the silicon substrate.Comment: 6 pages, 6 figures, proceeding for the INFOS2005 conference
(http://www.imec.be/infos/
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
Effects of Al doping on the structural and electronic properties of Mg(1-x)Al(x)B2
We have studied the structural and electronic properties of Mg(1-x)Al(x)B2
within the Virtual Crystal Approximation (VCA) by means of first-principles
total-energy calculations. Results for the lattice parameters, the electronic
band structure, and the Fermi surface as a function of Al doping for 0<x<0.6
are presented. The ab initio VCA calculations are in excellent agreement with
the experimentally observed change in the lattice parameters of Al doped MgB2.
The calculations show that the Fermi surface associated with holes a the boron
planes collapses gradually with aluminum doping and vanishes for x=0.56. In
addition, an abrupt topological change in the sigma-band Fermi surface was
found for x=0.3. The calculated hole density correlates closely with existing
experimental data for Tc(x), indicating that the observed loss of
superconductivity in Mg(1-x)Al(x)B2 is a result of hole bands filling.Comment: 4 pages (revtex) and 4 figures (postscript
Optical properties of structurally-relaxed Si/SiO superlattices: the role of bonding at interfaces
We have constructed microscopic, structurally-relaxed atomistic models of
Si/SiO superlattices. The structural distortion and oxidation-state
characteristics of the interface Si atoms are examined in detail. The role
played by the interface Si suboxides in raising the band gap and producing
dispersionless energy bands is established. The suboxide atoms are shown to
generate an abrupt interface layer about 1.60 \AA thick. Bandstructure and
optical-absorption calculations at the Fermi Golden rule level are used to
demonstrate that increasing confinement leads to (a) direct bandgaps (b) a blue
shift in the spectrum, and (c) an enhancement of the absorption intensity in
the threshold-energy region. Some aspects of this behaviour appear not only in
the symmetry direction associated with the superlattice axis, but also in the
orthogonal plane directions. We conclude that, in contrast to Si/Ge, Si/SiO
superlattices show clear optical enhancement and a shift of the optical
spectrum into the region useful for many opto-electronic applications.Comment: 11 pages, 10 figures (submitted to Phys. Rev. B
Structural and magnetic properties of Fe/ZnSe(001) interfaces
We have performed first principles electronic structure calculations to
investigate the structural and magnetic properties of Fe/ZnSe(001) interfaces.
Calculations involving full geometry optimizations have been carried out for a
broad range of thickness of Fe layers(0.5 monolayer to 10 monolayers) on top of
a ZnSe(001) substrate. Both Zn and Se terminated interfaces have been explored.
Total energy calculations show that Se segregates at the surface which is in
agreement with recent experiments.
For both Zn and Se terminations, the interface Fe magnetic moments are higher
than the bulk bcc Fe moment.
We have also investigated the effect of adding Fe atoms on top of a
reconstructed ZnSe surface to explore the role of reconstruction of
semiconductor surfaces in determining properties of metal-semiconductor
interfaces. Fe breaks the Se dimer bond formed for a Se-rich (2x1)
reconstructed surface. Finally, we looked at the reverse growth i.e. growth of
Zn and Se atoms on a bcc Fe(001) substrate to investigate the properties of the
second interface of a magnetotunnel junction. The results are in good agreement
with the theoretical and experimental results, wherever available.Comment: 7 pages, 8 figures, accepted for publication in PR
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.
Large Orbital Magnetic Moment and Coulomb Correlation effects in FeBr2
We have performed an all-electron fully relativistic density functional
calculation to study the magnetic properties of FeBr2. We show for the first
time that the correlation effect enhances the contribution from orbital degrees
of freedom of electrons to the total magnetic moment on Fe as
opposed to common notion of nearly total quenching of the orbital moment on
Fe site. The insulating nature of the system is correctly predicted when
the Hubbard parameter U is included. Energy bands around the gap are very
narrow in width and originate from the localized Fe-3 orbitals, which
indicates that FeBr2 is a typical example of the Mott insulator.Comment: 4 pages, 3 figures, revtex4, PRB accepte
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