194 research outputs found
Migration of Mg and other interstitial metal dopants in GaN
The minimum energy paths for the migration of interstitial Mg in wurtzite GaN
are studied through density functional calculations. The study also comprises
Li, Na, and Be dopants to examine the dependence on size and charge of the
dopant species. In all cases considered, the impurities diffuse like ions
without any tendency of localizing charge. Li, Mg, and to some extent Na,
diffuse almost isotropically in GaN, with average diffusion barriers of 1.1,
2.1, and 2.5 eV, respectively. Instead Be shows a marked anisotropy with energy
barriers of 0.76 and 1.88 eV for diffusion paths perpendicular and parallel to
the c-axis. The diffusion barrier generally increases with ionic charge and
ionic radius, but their interplay is not trivial. The calculated migration
barrier for Mg is consistent with the values estimated in a recent beta-
emission channeling experiment
Metal adatoms on graphene and hexagonal boron nitride: Towards the rational design of self-assembly templates
Periodically corrugated epitaxial graphene and hexagonal boron nitride (h-BN)
on metallic substrates are considered as perspective templates for the
self-assembly of nanoparticles arrays. By using first-principles calculations,
we determine binding energies and diffusion activation barriers of metal
adatoms on graphene and h-BN. The observed chemical trends can be understood in
terms of the interplay between charge transfer and covalent bonding involving
the adatom d electrons. We further investigate the electronic effects of the
metallic substrate and find that periodically corrugated templates based on
graphene in combination with strong interactions at the metal/graphene
interface are the most suitable for the self-assembly of highly regular
nanoparticle arrays.Comment: 5 pages, 3 figures, 1 tabl
Magnetoresistive junctions based on epitaxial graphene and hexagonal boron nitride
We propose monolayer epitaxial graphene and hexagonal boron nitride (h-BN) as
ultimate thickness covalent spacers for magnetoresistive junctions. Using a
first-principles approach, we investigate the structural, magnetic and spin
transport properties of such junctions based on structurally well defined
interfaces with (111) fcc or (0001) hcp ferromagnetic transition metals. We
find low resistance area products, strong exchange couplings across the
interface, and magnetoresistance ratios exceeding 100% for certain chemical
compositions. These properties can be fine tuned, making the proposed junctions
attractive for nanoscale spintronics applications.Comment: 5 page
Liquid Water through Density-Functional Molecular Dynamics: Plane-Wave vs Atomic-Orbital Basis Sets
We determine and compare structural, dynamical, and electronic properties of
liquid water at near ambient conditions through density-functional molecular
dynamics simulations, when using either plane-wave or atomic-orbital basis
sets. In both frameworks, the electronic structure and the atomic forces are
self-consistently determined within the same theoretical scheme based on a
nonlocal density functional accounting for van der Waals interactions. The
overall properties of liquid water achieved within the two frameworks are in
excellent agreement with each other. Thus, our study supports that
implementations with plane-wave or atomic-orbital basis sets yield equivalent
results and can be used indiscriminately in study of liquid water or aqueous
solutions
Effect of Metal Element in Catalytic Growth of Carbon Nanotubes
Using first principles calculations, we model the chemical vapor deposition
(CVD) growth of carbon nanotubes (CNT) on nanoparticles of late transition (Ni,
Pd, Pt) and coinage (Cu, Ag, Au) metals. The process is analyzed in terms of
the binding of mono- and diatomic carbon species, their diffusion pathways, and
the stability of the growing CNT. We find that the diffusion pathways can be
controlled by the choice of the catalyst and the carbon precursor. Binding of
the CNT through armchair edges is more favorable than through zigzag ones, but
the relative stability varies significantly among the metals. Coinage metals,
in particular Cu, are found to favor CVD growth of CNTs at low temperatures and
with narrow chirality distributions.Comment: Phys. Rev. Lett., accepte
Band-edge problem in the theoretical determination of defect energy levels: the O vacancy in ZnO as a benchmark case
Calculations of formation energies and charge transition levels of defects
routinely rely on density functional theory (DFT) for describing the electronic
structure. Since bulk band gaps of semiconductors and insulators are not well
described in semilocal approximations to DFT, band-gap correction schemes or
advanced theoretical models which properly describe band gaps need to be
employed. However, it has become apparent that different methods that reproduce
the experimental band gap can yield substantially different results regarding
charge transition levels of point defects. We investigate this problem in the
case of the (+2/0) charge transition level of the O vacancy in ZnO, which has
attracted considerable attention as a benchmark case. For this purpose, we
first perform calculations based on non-screened hybrid density functionals,
and then compare our results with those of other methods. While our results
agree very well with those obtained with screened hybrid functionals, they are
strikingly different compared to those obtained with other band-gap corrected
schemes. Nevertheless, we show that all the different methods agree well with
each other and with our calculations when a suitable alignment procedure is
adopted. The proposed procedure consists in aligning the electron band
structure through an external potential, such as the vacuum level. When the
electron densities are well reproduced, this procedure is equivalent to an
alignment through the average electrostatic potential in a calculation subject
to periodic boundary conditions. We stress that, in order to give accurate
defect levels, a theoretical scheme is required to yield not only band gaps in
agreement with experiment, but also band edges correctly positioned with
respect to such a reference potential
Charge state of the O molecule during silicon oxidation through hybrid functional calculations
We study the charge state of the diffusing O molecule during silicon
oxidation through hybrid functional calculations. We calculate charge
transition levels of O in bulk SiO and use theoretical band offsets to
align these levels with respect to the Si band edges. To overcome the band-gap
problem of semilocal density fuctionals, we employ hybrid functionals with both
predefined and empirically adjusted mixing coefficients. We find that the
charge transition level in bulk SiO occurs at 1.1 eV
above the silicon conduction band edge, implying that the O molecule
diffuses through the oxide in the neutral charge state. While interfacial
effects concur to lower the charge transition level, our estimates suggest that
the neutral charge state persists until silicon oxidation.Comment: 4 pages, 3 figure
Hubbard through polaronic defect states
Since the preliminary work of Anisimov and co-workers, the Hubbard corrected
DFT+ functional has been used for predicting properties of correlated
materials by applying on-site effective Coulomb interactions to specific
orbitals. However, the determination of the Hubbard parameter has remained
under intense discussion despite the multitude of approaches proposed. Here, we
define a selection criterion based on the use of polaronic defect states for
the enforcement of the piecewise linearity of the total energy upon electron
occupation. The values of determined in this way are found to be robust
upon variation of the considered state. The corresponding electronic and
structural properties are in good agreement with results from piecewise linear
hybrid functionals. In particular, defect formation energies are well
reproduced, thereby validating the energetics achieved with our selection
criterion. It is emphasized that the selection of should be based on
physical properties directly associated with the orbitals to which is
applied, rather than on more global properties such as band gaps. For
comparison, we also determine through a well-established linear response
scheme finding noticeably different values of and consequently different
formation energies. Possible origins of these discrepancies are discussed. As
case studies, we consider the self-trapped electron in BiVO, the
self-trapped hole in MgO, the Li-trapped hole in MgO, and the Al-trapped hole
in -SiO.Comment: 7 pages, 4 figure
Carbon rehybridization at the graphene/SiC(0001) interface: Effect on stability and atomic-scale corrugation
We address the energetic stability of the graphene/SiC(0001) interface and
the associated binding mechanism by studying a series of low-strain
commensurate interface structures within a density functional scheme. Among the
structures with negligible strain, the 6\surd3\times6\surd3 R30{\deg} SiC
periodicity shows the lowest interface energy, providing a rationale for its
frequent experimental observation. The interface stability is driven by the
enhanced local reactivity of the substrate-bonded graphene atoms undergoing
sp2-to-sp3 rehybridization (pyramidalization). By this mechanism, relaxed
structures of higher stability exhibit more pronounced graphene corrugations at
the atomic scale
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