It is argued that topological disorder in amorphous solids can be described by local strains related to local reference crystals and local rotations. An intuitive localization criterion is formulated from this point of view. The Inverse Participation Ratio and the location of mobility edges in band tails is directly related to the character of the disorder potential in amorphous solid, the coordination number, the transition integral and the nodes of wave functions of the corresponding reference crystal. The dependence of the decay rate of band tails on temperature and static disorder are derived. \textit{Ab initio} simulations on a-Si and experiments on a-Si:H are compared to these predictions.
We investigated the microscopic and electronic structures amorphous oxide semiconductors InGaZnO$_{4}$ (a-IGZO) and the role of O-deficiency through the first-principle calculations. The structure of the amorphous oxide is complicated by the admixture of many different kinds of substructures, however it is surprisingly found that the band tail states, which are well-known to be present in the amorphous semiconductors, are few generated for the conduction band minimum (CBM). The electronic structure around CBM is little affected by the disorder and also by the O-deficiency. Free electron carrie…
We present a simple model of the bimolecular charge carrier recombination in polar amorphous organic semiconductors where the dominant part of the energetic disorder is provided by permanent dipoles and show that the recombination rate constant could be much smaller than the corresponding Langevin rate constant. The reason for the strong decrease of the rate constant is the long range spatial correlation of the random energy landscape in amorphous dipolar materials, without spatial correlation even strong disorder does not modify the Langevin rate constant. Our study shows that the significant…
We consider the bimolecular charge carrier recombination in amorphous organic semiconductors having a special kind of energetic disorder where energy levels for electrons and holes at a given transport site move in the same direction with the variation of some disorder governing parameter (the parallel disorder). This particular kind of disorder could be found in materials where the dominant part of the energetic disorder is provided by the conformational disorder. Contrary to the recently studied case of electrostatic disorder, the conformational disorder, if spatially correlated, leads to th…
The excited holes occupying the valence band tail states in amorphous oxide semiconductors are found to induce formation of meta-stable O$_2^{2-}$ peroxide defects. The valence band tail states are at least partly characterized by the O-O ppσ* molecular orbital, and the localized-hole-mediated lattice instability results in the formation of the peroxide defects. Along with the O-O bond formation, the ppσ* state is heightened up into the conduction bands, and two electrons are accordingly doped in the electronic ground state. The energy barrier from the O$_2^{2-}$ peroxide state to the normal d…
The article describes an experimental method that allows to estimate the inhomogeneous and homogeneous linewidths of the photoluminescence band of a point defect in an amorphous solid. We performed low temperature time-resolved luminescence measurements on two defects chosen as model systems for our analysis: extrinsic Oxygen Deficient Centers (ODC(II)) in amorphous silica and F+ 3 centers in crystalline Lithium Fluoride. Measurements evidence that only defects embedded in the amorphous matrix feature a dependence of the radiative decay lifetime on the emission energy and a time dependence of …
This paper addresses a difficult inverse problem that involves the reconstruction of a three-dimensional model of tetrahedral amorphous semiconductors via inversion of diffraction data. By posing the material-structure determination as a multi-objective optimization program, it has been shown that the problem can be solved accurately using a few structural constraints, but no total-energy functionals/forces, which describe the local chemistry of amorphous networks. The approach yields highly realistic models of amorphous silicon, with no or only a few coordination defects ($\le$ 1%), a narrow …
Sound attenuation in low temperature amorphous solids originates from their disordered structure. However, its detailed mechanism is still being debated. Here we analyze sound attenuation starting directly from the microscopic equations of motion. We derive an exact expression for the zero-temperature sound damping coefficient. We verify that the sound damping coefficients calculated from our expression agree very well with results from independent simulations of sound attenuation. The small wavevector analysis of our expression shows that sound attenuation is primarily determined by the non-a…
Rapidly cooling a liquid may result in a glass transition, creating an amorphous solid whose shear and bulk moduli are finite. Even when done with constant density, these resulting moduli depend strongly on the rate of cooling. Understanding this phenomenon calls for analyzing separately the "Born term" that exists also in perfectly ordered materials and the contributions of the "excess modes" that result from glassy disorder. We show that the Born term is very insensitive to the cooling rate, and all the variation in the shear modulus is due to the excess modes. We argue that this approach pr…
We report the results of a large-scale modelling study of radiation damage effects in the nuclear waste form zirconolite. We particularly focus on the effects of radiation damage in amorphous zirconolite and have developed a new way to analyse the damaged structure in terms of local coordination statistics. On the basis of this analysis, we find that the amorphous structure responds to radiation damage differently from the crystal. Amorphous zirconolite is found to be "softer" than crystalline zirconolite with a much larger number of atoms becoming displaced and changing coordination during a …
The synthesis of wafer-scale two-dimensional amorphous carbon monolayers has been recently demonstrated. This material presents useful properties when integrated as coating of metals, semiconductors or magnetic materials, such as enabling efficient atomic layer deposition and hence fostering the development of ultracompact technologies. Here we propose a characterization of how the structural degree of amorphousness of such carbon membranes could be controlled by the crystal growth temperature. We also identify how energy is dissipated in this material by a systematic analysis of emerging vibr…
Glasses are known to exhibit quantitative universalities at low temperatures, the most striking of which is the ultrasonic attenuation coefficient 1/Q. In this work we develop a theory of coupled generic blocks with a certain randomness property to show that universality emerges essentially due to the interactions between elastic blocks, regardless of their microscopic nature.
We propose a simple approach to investigate the structural relaxation time and glass transition of amorphous drugs. Amorphous materials are modeled as a set of equal sized hard spheres. The structural relaxation time over many decades in hard sphere fluids is theoretically calculated using the Elastically Collective Nonlinear Langevin Equation theory associated with Kramer's theory. Then, a new thermal mapping from a real material to an effective hard sphere fluid provides temperature-dependent relaxation time, which can compare to experiments. Numerical results quantitatively agree with previ…
The behavior of shear-oscillated amorphous materials is studied using a coarse-grained model. Samples are prepared at different degrees of annealing and then subject to athermal and quasistatic oscillatory deformations at various fixed amplitudes. The steady-state reached after several oscillations is fully determined by the initial preparation and the oscillation amplitude, as seen from stroboscopic stress and energy measurements. Under small oscillations, poorly annealed materials display shear-annealing, while ultra-stabilized materials are insensitive to them. Yet, beyond a critical oscill…
Here, we present the measurements of $R_H$ in a series of $Ti_xSi_{100-x}$ amorphous reaching the critical concentration, $x_c\approx9-9.5$. For $x\geq17$, the Hall coefficient displays the behavior predicted by the perturbation theory, $R_H^{-1}\left(T\right)=R_H^{-1}\left(0\right)+bT^{1/2}$, which extends up to the temperature 150 K. The temperature dependence gets stronger in alloys with lower $x$; $R_H\left(0\right)$ diverges at $x_c$ displaying critical behavior. We used the combined conductivity and Hall coefficient data for alloys with high Ti content to test the theories of quantum cor…
Physics-Informed Glass-Structure Descriptors for Assessing the Intrinsic Reactivity of Mixed Amorphous-Crystalline Precursors in Alkali-Activated Materials
We propose a framework that unifies the description of light transport in three-dimensional amorphous dielectric materials that exhibit both localization and a photonic bandgap. To this end, we argue that coherent reflection near and in the bandgap attenuates the generation of diffuse or localized photons. Using the self-consistent theory of localization and considering the density of states of photons, we can quantitatively describe all transport regimes: Transparency, light diffusion, localization, and bandgap. Comparing the model with numerical data on optical transport in hyperuniform diel…
We discuss the strain dependence of the acoustic properties of amorphous metals in both normal and superconducting states, in the temperature range 0.1 mK $ \le T \le 1 $K. A crossover is found when the strain energy is of the order of the effective interaction energy between tunneling systems at the corresponding temperature. Our results provide clear evidence for the interaction between tunneling systems, whose energy is in quantitative agreement with theoretical expectations, and reveal that without the knowledge of the corresponding strain dependences, the measured temperature dependences …
An approximation scheme for model disordered solids is proposed that leads to the fully analytical evaluation of the elastic constants under explicit account of the inhomogeneity (nonaffinity) of the atomic displacements. The theory is in quantitative agreement with simulations for central-force systems and predicts the vanishing of the shear modulus at the isostatic point with the linear law μ ~ (z - 2d), where z is the coordination number. The vanishing of rigidity at the isostatic point is shown to be a consequence of the canceling out of positive affine and negative nonaffine terms.
We report specific heat and thermal conductivity of gadolinium- and yttrium-doped amorphous silicon thin films measured using silicon-nitride membrane-based microcalorimeters. Addition of gadolinium or yttrium to the amorphous silicon network reduces the thermal conductivity over a wide temperature range while significantly increasing the specific heat. This result indicates that a large number of non-propagating states are added to the vibrational spectrum that are most likely caused either by localized vibration of the dopant atom in a Si cage, or softening of the material forming the cage s…
We show that viscoelastic effects play a crucial role in the damping of vibrational modes in harmonic amorphous solids. The relaxation of a given plane wave is described by a memory function of a semi-infinite one-dimensions mass-spring chain. The initial vibrational energy spreads from the first site of the chain to infinity. In the beginning of the chain, there is a barrier, which significantly reduces the decay of vibrational energy below the Ioffe-Regel frequency. To obtain the parameters of the chain, we present a numerically stable method, based on the Chebyshev expansion of the local vi…
Amorphous solids display numerous universal features in their mechanics, structure, and response. Current models assume heterogeneity in mesoscale elastic properties, but require fine-tuning in order to quantitatively explain vibrational properties. A complete model should derive the magnitude and character of elastic heterogeneity from an initially structureless medium, through a model of the quenching process during which the temperature is rapidly lowered and the solid is formed. Here we propose a field-theoretic model of a quench, and compute structural, mechanical, and vibrational observa…
The phonon spectra of solids, described through the measurable vibrational density of states (VDOS), provide a wealth of information about the underlying atomic structure and bonding, and they determine fundamental macroscopic properties such as specific heat, thermal conductivity and superconductivity. In amorphous solids, structural disorder generates a number of poorly understood phenomena that are absent in crystals. Starting from an effective field theory description which accounts for disorder in terms of momentum diffusion, we provide a unified theoretical description of the VDOS of amo…
We propose a simple route to evaluate the static structure, in terms of average coordination, of completely disordered solids with spherical constituents, from ca. 55% volume fraction up to random close packing, in the absence of structural heterogeneities. Based on the current understanding, according to which the structure-determining interaction in amorphous solids is the hard-core repulsion while weaker, longer-range interactions are mere perturbations, the model yields the average coordination in the solid as a result of a hyperquenching process where the instantaneous structure of the pr…
A random matrix approach is used to analyze the vibrational properties of amorphous solids. We investigated a dynamical matrix M=AA^T with non-negative eigenvalues. The matrix A is an arbitrary real NxN sparse random matrix with n independent non-zero elements in each row. The average values <A_{ij}>=0 and dispersion <A_{ij}^2>=V^2 for all non-zero elements. The density of vibrational states g(w) of the matrix M for N,n >> 1 is given by the Wigner quarter circle law with radius independent of N. We argue that for n^2 << N this model can be used to describe the interaction of atoms in amorphous…
Amorphous solids have excess soft modes in addition to the phonon modes described by the Debye theory. Recent numerical results show that if the phonon modes are carefully removed, the density of state of the excess soft modes exhibit universal quartic scaling, independent of the interaction potential, preparation protocol, and spatial dimensions. We hereby provide a theoretical framework to describe this universal scaling behavior. For this purpose, we extend the mean-field theory to include the effects of finite dimensional fluctuation. Based on a semi-phenomenological argument, we show that…
We present a mathematical description of amorphous solid deformation and plasticity by extending the concept of instantaneous normal modes (INMs) to deformed systems, which allows us to retain the effect of strain on the vibrational density of states (VDOS). Starting from the nonaffine lattice dynamics (NALD) description of elasticity and viscoelasticity of glasses, we formulate the linear response theory up to large deformations by considering the strain-dependent tangent modulus at finite values of shear strain. The (nonaffine) tangent shear modulus is computed from the vibrational density o…
Amorphous solids appear to react elastically to small external strains, but in contrast to ideal elastic media, plastic responses abound immediately, at any value of the strain. Such plastic responses are quasi-localized in nature, with the ``cheapest" one being a quadrupolar source. The existence of such plastic responses results in {\em screened elasticity} in which strains and stresses can either quantitatively or qualitatively differ from the un-screened theory, depending on the specific screening mechanism. Here we offer a theory of such screening effects by plastic quadrupoles, dipoles a…
