461 research outputs found
Energetics of intrinsic point defects in ZrSiO
Using first principles calculations we have studied the formation energies,
electron and hole affinities, and electronic levels of intrinsic point defects
in zircon. The atomic structures of charged interstitials, vacancies, Frenkel
pairs and anti-site defects are obtained. The limit of high concentration of
point defects, relevant for the use of this material in nuclear waste
immobilization, was studied with a variable lattice relaxation that can
simulate the swelling induced by radiation damage. The limit of low
concentration of defects is simulated with larger cells and fixed lattice
parameters. Using known band offset values at the interface of zircon with
silicon, we analyze the foreseeable effect of the defects on the electronic
properties of zircon used as gate in metal-oxide-semiconductor devices.Comment: preprint 16 pages, 4 figures, and 5 table
Structural and configurational properties of nanoconfined monolayer ice from first principles
Understanding the structural tendencies of nanoconfined water is of great interest for nanoscience and biology, where nano/micro-sized objects may be separated by very few layers of water. Here we investigate the properties of ice confined to a quasi-2D monolayer by a featureless, chemically neutral potential, in order to characterize its intrinsic behaviour. We use density-functional theory simulations with a non-local van der Waals density functional. An ab initio random structure search reveals all the energetically competitive monolayer configurations to belong to only two of the previously-identified families, characterized by a square or honeycomb hydrogen-bonding network, respectively. We discuss the modified ice rules needed for each network, and propose a simple point dipole 2D lattice model that successfully explains the energe tics of the square configurations. All identified stable phases for both networks are found to be non-polar (but with a topologically non-trivial texture for the square) and, hence, non-ferroelectric, in contrast to previous predictions from a five-site empirical force-field model. Our results are in good agreement with very recently reported experimental observations.This work was partly funded by grants FIS2012-37549-C05 from the Spanish Ministry of Science, and Exp. 97/14 (Wet Nanoscopy) from the Programa Red Guipuzcoana de Ciencia, Tecnología e Innovación, Diputación Foral de Gipuzkoa. We thank Richard Korytár and Javier Junquera for their work on the SIESTA interface to Wannier90, and Raffaele Resta and M.-V. Fernández-Serra for useful discussions. The calculations were performed on the arina HPC cluster (Universidad del País Vasco/Euskal Herriko Unibertsitatea, Spain). SGIker (UPV/EHU, MICINN, GV/EJ, ERDF and ESF) support is gratefully acknowledged
Ferrodistortive instability at the (001) surface of half-metallic manganites
We present the structure of the fully relaxed (001) surface of the
half-metallic manganite La0.7Sr0.3MnO3, calculated using density functional
theory within the generalized gradient approximation (GGA). Two relevant
ferroelastic order parameters are identified and characterized: The tilting of
the oxygen octahedra, which is present in the bulk phase, oscillates and
decreases towards the surface, and an additional ferrodistortive Mn
off-centering, triggered by the surface, decays monotonically into the bulk.
The narrow d-like energy band that is characteristic of unrelaxed manganite
surfaces is shifted down in energy by these structural distortions, retaining
its uppermost layer localization. The magnitude of the zero-temperature
magnetization is unchanged from its bulk value, but the effective spin-spin
interactions are reduced at the surface.Comment: 4 pages, 2 figure
Intrinsic point defects and volume swelling in ZrSiO4 under irradiation
The effects of high concentration of point defects in crystalline ZrSiO4 as
originated by exposure to radiation, have been simulated using first principles
density functional calculations. Structural relaxation and vibrational studies
were performed for a catalogue of intrinsic point defects, with different
charge states and concentrations. The experimental evidence of a large
anisotropic volume swelling in natural and artificially irradiated samples is
used to select the subset of defects that give similar lattice swelling for the
concentrations studied, namely interstitials of O and Si, and the anti-site
Zr(Si), Calculated vibrational spectra for the interstitials show additional
evidence for the presence of high concentrations of some of these defects in
irradiated zircon.Comment: 9 pages, 7 (color) figure
Structural relaxations in electronically excited poly(para-phenylene)
Structural relaxations in electronically excited poly(para-phenylene) are
studied using many-body perturbation theory and density-functional-theory
methods. A sophisticated description of the electron-hole interaction is
required to describe the energies of the excitonic states, but we show that the
structural relaxations associated with exciton formation can be obtained quite
accurately within a constrained density-functional-theory approach. We find
that the structural relaxations in the low-energy excitonic states extend over
about 8 monomers, leading to an energy reduction of 0.22 eV and a Stokes shift
of 0.40 eV.Comment: 4 pages, 3 figure
Geometry and quantum delocalization of interstitial oxygen in silicon
The problem of the geometry of interstitial oxygen in silicon is settled by
proper consideration of the quantum delocalization of the oxygen atom around
the bond-center position. The calculated infrared absorption spectrum accounts
for the 517 and 1136 cm bands in their position, character, and isotope
shifts. The asymmetric lineshape of the 517 cm peak is also well
reproduced. A new, non-infrared-active, symmetric-stretching mode is found at
596 cm. First-principles calculations are presented supporting the
nontrivial quantum delocalization of the oxygen atom.Comment: uuencoded, compressed postscript file for the whole. 4 pages (figures
included), accepted in PR
Surface energy and stability of stress-driven discommensurate surface structures
A method is presented to obtain {\it ab initio} upper and lower bounds to
surface energies of stress-driven discommensurate surface structures, possibly
non-periodic or exhibiting very large unit cells. The instability of the
stressed, commensurate parent of the discommensurate structure sets an upper
bound to its surface energy; a lower bound is defined by the surface energy of
an ideally commensurate but laterally strained hypothetical surface system. The
surface energies of the phases of the Si(111):Ga and Ge(111):Ga systems and the
energies of the discommensurations are determined within eV.Comment: 4 pages RevTeX. 2 Figures not included. Ask for a hard copy (through
regular mail) to [email protected]
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