40 research outputs found
A new type of charged defect in amorphous chalcogenides
We report on density-functional-based tight-binding (DFTB) simulations of a
series of amorphous arsenic sulfide models. In addition to the charged
coordination defects previously proposed to exist in chalcogenide glasses, a
novel defect pair, [As4]--[S3]+, consisting of a four-fold coordinated arsenic
site in a seesaw configuration and a three-fold coordinated sulfur site in a
planar trigonal configuration, was found in several models. The
valence-alternation pairs S3+-S1- are converted into [As4]--[S3]+ pairs under
HOMO-to-LUMO electronic excitation. This structural transformation is
accompanied by a decrease in the size of the HOMO-LUMO band gap, which suggests
that such transformations could contribute to photo-darkening in these
materials.Comment: 5 pages, 2 figure
Simulation of physical properties of the chalcogenide glass As2S3 using a density-functional-based tight-binding method
We have used a density-functional-based tight-binding method in order to create structural models of the canonical chalcogenide glass, amorphous As2S3. The models range from one containing defects that are both chemical (homopolar bonds) and topological (valence-alternation pairs) in nature to one that is defect-free (stoichiometric). The structural, vibrational, and electronic properties of the simulated models are in good agreement with experimental data where available. The electronic densities of states obtained for all models show clean optical band gaps. A certain degree of electron-state localization at the band edges is observed for all models, which suggests that photoinduced phenomena in chalcogenide glasses may not necessarily be attributed to the excitation of defects of only one particular kind
Influence of copper on the electronic properties of amorphous chalcogenides
We have studied the influence of alloying copper with amorphous arsenic
sulfide on the electronic properties of this material. In our
computer-generated models, copper is found in two-fold near-linear and
four-fold square-planar configurations, which apparently correspond to Cu(I)
and Cu(II) oxidation states. The number of overcoordinated atoms, both arsenic
and sulfur, grows with increasing concentration of copper. Overcoordinated
sulfur is found in trigonal planar configuration, and overcoordinated
(four-fold) arsenic is in tetrahedral configuration. Addition of copper
suppresses the localization of lone-pair electrons on chalcogen atoms, and
localized states at the top of the valence band are due to Cu 3d orbitals.
Evidently, these additional Cu states, which are positioned at the same
energies as the states due to ([As4]-)-([S_3]+) pairs, are responsible for
masking photodarkening in Cu chalcogenides
On the decay of Burgers turbulence
This work is devoted to the decay ofrandom solutions of the unforced Burgers
equation in one dimension in the limit of vanishing viscosity. The initial
velocity is homogeneous and Gaussian with a spectrum proportional to at
small wavenumbers and falling off quickly at large wavenumbers. In physical
space, at sufficiently large distances, there is an ``outer region'', where the
velocity correlation function preserves exactly its initial form (a power law)
when is not an even integer. When the spectrum, at long times, has
three scaling regions : first, a region at very small \ms1 with a
time-independent constant, stemming from this outer region, in which the
initial conditions are essentially frozen; second, a region at
intermediate wavenumbers, related to a self-similarly evolving ``inner region''
in physical space and, finally, the usual region, associated to the
shocks. The switching from the to the region occurs around a wave
number , while the switching from to
occurs around (ignoring logarithmic
corrections in both instances). The key element in the derivation of the
results is an extension of the Kida (1979) log-corrected law for the
energy decay when to the case of arbitrary integer or non-integer .
A systematic derivation is given in which both the leading term and estimates
of higher order corrections can be obtained. High-resolution numerical
simulations are presented which support our findings.Comment: In LaTeX with 11 PostScript figures. 56 pages. One figure contributed
by Alain Noullez (Observatoire de Nice, France
Universal Features of Terahertz Absorption in Disordered Materials
Using an analytical theory, experimental terahertz time-domain spectroscopy
data and numerical evidence, we demonstrate that the frequency dependence of
the absorption coupling coefficient between far-infrared photons and atomic
vibrations in disordered materials has the universal functional form, C(omega)
= A + B*omega^2, where the material-specific constants A and B are related to
the distributions of fluctuating charges obeying global and local charge
neutrality, respectively.Comment: 5 pages, 3 fig
Nature of vibrational eigenmodes in topologically disordered solids
We use a local projectional analysis method to investigate the effect of
topological disorder on the vibrational dynamics in a model glass simulated by
molecular dynamics. Evidence is presented that the vibrational eigenmodes in
the glass are generically related to the corresponding eigenmodes of its
crystalline counterpart via disorder-induced level-repelling and hybridization
effects. It is argued that the effect of topological disorder in the glass on
the dynamical matrix can be simulated by introducing positional disorder in a
crystalline counterpart.Comment: 7 pages, 6 figures, PRB, to be publishe
Extended point defects in crystalline materials: Ge and Si
B diffusion measurements are used to probe the basic nature of
self-interstitial 'point' defects in Ge. We find two distinct self-interstitial
forms - a simple one with low entropy and a complex one with entropy ~30 k at
the migration saddle point. The latter dominates diffusion at high temperature.
We propose that its structure is similar to that of an amorphous pocket - we
name it a 'morph'. Computational modelling suggests that morphs exist in both
self-interstitial and vacancy-like forms, and are crucial for diffusion and
defect dynamics in Ge, Si and probably many other crystalline solids