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

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 $k^n$ at small wavenumbers $k$ 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 $n$ is not an even integer. When $1<n<2$ the spectrum, at long times, has three scaling regions : first, a $|k|^n$ region at very small $k$\ms1 with a time-independent constant, stemming from this outer region, in which the initial conditions are essentially frozen; second, a $k^2$ region at intermediate wavenumbers, related to a self-similarly evolving ``inner region'' in physical space and, finally, the usual $k^{-2}$ region, associated to the shocks. The switching from the $|k|^n$ to the $k^2$ region occurs around a wave number $k_s(t) \propto t^{-1/[2(2-n)]}$, while the switching from $k^2$ to $k^{-2}$ occurs around $k_L(t)\propto t^{-1/2}$ (ignoring logarithmic corrections in both instances). The key element in the derivation of the results is an extension of the Kida (1979) log-corrected $1/t$ law for the energy decay when $n=2$ to the case of arbitrary integer or non-integer $n>1$. 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

Relationship between dynamical heterogeneities and stretched exponential relaxation

We identify the dynamical heterogeneities as an essential prerequisite for stretched exponential relaxation in dynamically frustrated systems. This heterogeneity takes the form of ordered domains of finite but diverging lifetime for particles in atomic or molecular systems, or spin states in magnetic materials. At the onset of the dynamical heterogeneity, the distribution of time intervals spent in such domains or traps becomes stretched exponential at long time. We rigorously show that once this is the case, the autocorrelation function of the renewal process formed by these time intervals is also stretched exponential at long time.Comment: 8 pages, 4 figures, submitted to PR

The global picture of self-similar and not self-similar decay in Burgers Turbulence

This paper continue earlier investigations on the decay of Burgers turbulence in one dimension from Gaussian random initial conditions of the power-law spectral type $E_0(k)\sim|k|^n$. Depending on the power $n$, different characteristic regions are distinguished. The main focus of this paper is to delineate the regions in wave-number $k$ and time $t$ in which self-similarity can (and cannot) be observed, taking into account small-$k$ and large-$k$ cutoffs. The evolution of the spectrum can be inferred using physical arguments describing the competition between the initial spectrum and the new frequencies generated by the dynamics. For large wavenumbers, we always have $k^{-2}$ region, associated to the shocks. When $n$ is less than one, the large-scale part of the spectrum is preserved in time and the global evolution is self-similar, so that scaling arguments perfectly predict the behavior in time of the energy and of the integral scale. If $n$ is larger than two, the spectrum tends for long times to a universal scaling form independent of the initial conditions, with universal behavior $k^2$ at small wavenumbers. In the interval $2<n$ the leading behaviour is self-similar, independent of $n$ and with universal behavior $k^2$ at small wavenumber. When $1<n<2$, the spectrum has three scaling regions : first, a $|k|^n$ region at very small $k$\ms1 with a time-independent constant, second, a $k^2$ region at intermediate wavenumbers, finally, the usual $k^{-2}$ region. In the remaining interval, $n<-3$ the small-$k$ cutoff dominates, and $n$ also plays no role. We find also (numerically) the subleading term $\sim k^2$ in the evolution of the spectrum in the interval $-3<n<1$. High-resolution numerical simulations have been performed confirming both scaling predictions and analytical asymptotic theory.Comment: 14 pages, 19 figure

Instantaneous frequency and amplitude identification using wavelets: Application to glass structure

This paper describes a method for extracting rapidly varying, superimposed amplitude- and frequency-modulated signal components. The method is based upon the continuous wavelet transform (CWT) and uses a new wavelet which is a modification to the well-known Morlet wavelet to allow analysis at high resolution. In order to interpret the CWT of a signal correctly, an approximate analytic expression for the CWT of an oscillatory signal is examined via a stationary-phase approximation. This analysis is specialized for the new wavelet and the results are used to construct expressions for the amplitude and frequency modulations of the components in a signal from the transform of the signal. The method is tested on a representative, variable-frequency signal as an example before being applied to a function of interest in our subject area - a structural correlation function of a disordered material - which immediately reveals previously undetected features.Comment: 9 pages, 19 figures; v1.04 higher quality diagrams, removed mathematica font requirement