The proposed algorithm by Philippe D'Arco et al. 2013 J. Phys.: Condens. Matter 25 355401 was not well compared with other possible solutions for symmetry independent configuration (SIC) generation. In this comment, three well known solutions of SIC searching are discussed: exhaustive explorations, pure random sampling and "symmetry imposed" approaches. It is shown, that the advantages of the algorithm published by Philippe D'Arco et al. are questionable.
By using very general arguments, we show that the entropy loss conjecture at the glass transition violates the second law of thermodynamics and must be rejected.
Comment on PRL v. 86, p. 5084 (2001) [cond-mat/0101016]. We point out that the authors' simulations are consistent with the known theory of steady-state solutions in this system.
We have examined the electrical transport in disordered molecular solids. It has been found that mobility is a function of electric field and temperature due to hopping conduction. Several theoretical models for charge transport in disordered solids have been debated over the role of spatial and energetic correlation in these systems and such correlations have been recently shown to explain the universal electric field dependence of mobility. We have compared and evaluated the applicability of different theoretically proposed models using very simple experimental results and based on our exten…
Site-occupancy disorder, defined as the non-periodic occupation of lattice sites in a crystal structure, is a ubiquitous phenomenon in solid-state physics and chemistry. Examples are mineral solid solutions, synthetic non-stoichiometric compounds and metal alloys. The experimental investigation of these materials using diffraction techniques only provides averaged information of their structure. However, many properties of interest in these solids are determined by the local geometry and degree of disorder, which escape an "average crystal" description, either from experiments or from theory. …
We propose here a first-principles, parameter free, real space method for the study of disordered extended defects in solids. We shall illustrate the power of the technique with an application to graphene sheets with randomly placed Stone-Wales defects and shall examine the signature of such random defects on the density of states as a function of their concentration. The technique is general enough to be applied to a whole class of systems with lattice translational symmetry broken not only locally but by extended defects and defect clusters. The real space approach will allow us to distingui…
The cohesive energies of solids calculated using mGLJ EOS proposed by Sun Jiuxun (Sun Jiuxun, J. Phys.: Condens. Matter 17, L103 (2005)) are seen to be erroneous. Also we observed that the thermodynamic properties calculated using the mGLJ potential diverge for materials whose pressure derivative of bulk modulus at equilibrium is less than 5. Thus the mGLJ potential cannot be used in liquid state theories and molecular simulations to obtain thermodynamic properties.
Recently first principles microscopic calculations, using the generalized gradient approximation, appeared for the solid mixed system $AgCl{_x}Br_{1-x}$ at various compositions. Here, we suggest a model that can estimate the compressibility of the mixed crystals in terms of the compressibilities of the end members alone. This model makes use of a single parameter, i.e., the compressibility of a defect volume, when considering the volume variation produced by the addition of a "foreign molecule" to a host crystal as a defect volume.
1. Introduction 2. Molecular dynamics simulation of amorphous carbon structures 3. Atomistic simulation of the bombardment process during the BEN phase of diamond CVD 4. Growth of amorphous silicon 5. One-dimensional hopping in disordered organic solids
The equation for the size strain plot methods reported by A. Khorsand Zak et al. (Solid State Sci. 13 (2011), 251) does not follow the dimensional homogeneity, consequently leading to an inaccurate estimation of the crystallite size and strain values of the materials under investigation and the dimensions of the obtained parameters. We also perceived an error in the values of crystallite size and strain reported by the authors using the size-strain plot method. We will discuss the importance of dimensional analysis and its repercussions on the estimated values and the units of parameters.
The low temperature universal properties in disordered and amorphous solids are considered. We introduce a model that includes two types of two level systems (TLSs), which, based on their local symmetry, interact weakly or strongly with the phonon field. This accounts well for the experimental results, and addresses some long-standing questions: the nature of the TLSs; the smallness and universality of the phonon attenuation, and the energy scale of $3$K below which universality is observed. Our model describes disordered lattices; we also discuss its application to amorphous solids.
Crystals and glasses exhibit fundamentally different heat conduction mechanisms: the periodicity of crystals allows for the excitation of propagating vibrational waves that carry heat, as first discussed by Peierls; in glasses, the lack of periodicity breaks Peierls' picture and heat is mainly carried by the coupling of vibrational modes, often described by a harmonic theory introduced by Allen and Feldman. Anharmonicity or disorder are thus the limiting factors for thermal conductivity in crystals or glasses; hitherto, no transport equation has been able to account for both. Here, we derive s…
Disordered hyperuniform (DHU) states are recently discovered exotic states of condensed matter. DHU systems are similar to liquids or glasses in that they are statistically isotropic and lack conventional long-range translational and orientational order. On the other hand, they completely suppress normalized infinite-wavelength density fluctuations like crystals, and in this sense possess a hidden long-range order. Very recently, there are several exciting discoveries of disordered hyperuniformity in solid-state materials, including amorphous carbon nanotubes, amorphous 2D silica, amorphous gr…
All solids yield under sufficiently high mechanical loads. Below yield, the mechanical responses of all disordered solids are nearly alike, but above yield every different disordered solid responds in its own way. Brittle systems can shatter without warning, like ordinary window glass, or exhibit strain localization prior to fracture, like metallic or polymeric glasses. Ductile systems, e.g. foams like shaving cream or emulsions like mayonnaise, can flow indefinitely with no strain localization. While there are empirical strategies for tuning the degree of strain localization, there is no fram…
The oxygen self-diffusion coefficient in UO${_2}$ has been recently studied [Cooper et al. Solid State Ionics 282 (2015) 26-30] over a range of pressures (0-10GPa) and temperatures (300-1900K) by combining molecular dynamics calculations with a thermodynamical model, the cBΩ model. A significant reduction in oxygen self-diffusion as a function of increasing hydrostatic pressure, and the associated increase in activation energy was identified. Here, we extend this study and find that the compressibility of the corresponding activation volume exceeds significantly the compressibility of the bulk…
Diffusion of atoms in solids is one of the most fundamental kinetic processes that ultimately governs many materials properties. Here, we report on a combined first-principles and kinetic Monte Carlo study of macroscopic diffusion properties of disordered Ti-Ta alloys over the entire composition range. Using simple cluster expansion model Hamiltonians parametrized on density functional theory data, we compute transport properties explicitly including local interactions between the two atomic species and compare them with the non-interacting diffusion model for disordered, random alloys. Surpri…
The old asperity model of Fuller and Tabor had demonstrated almost 50 years ago surprisingly good correlation with respect to quite a few experiments on the pull-off decay due to roughness of rubber spheres against roughened Perspex plates. We revisit here some features of the Fuller and Tabor model in view of the more recent theories and experiments, finding good correlation can be obtained only at intermediate resolutions, as perhaps in stylus profilometers. In general we confirm the predictions of the Persson & Tosatti and Bearing Area Model of Ciavarella, as stickiness depends largely on t…
Mechanical spectroscopy, i.e. cyclic deformations at varying frequencies, is used theoretically and numerically to measure dissipation in model glasses. From a normal mode analysis, we show that in the high-frequency THz regime where dissipation is harmonic, the quality factor (or loss angle) can be expressed analytically. This expression is validated through non-equilibrium molecular dynamics simulations applied to a model of amorphous silica (SiO$_2$). Dissipation is shown to arise from non-affine relaxations triggered by the applied strain through the excitation of vibrational eigenmodes th…
An oversight of several previous local density approximation (LDA) results appears to have led to an incomplete picture of the actual capability of density functional theory (DFT), with emphasis on LDA, to describe and to predict the band gaps of semiconductors [Phys. Rev. Lett. 105, 196403 (2010)]. LDA is portrayed as failing to describe the band gap of semiconductors. In light of the content of the literature, this characterization is misleading. These comments are intended to note some of these previous results and to provide an assessment of LDA capability that is drastically different fro…
Shearing a disordered or amorphous solid for many cycles with a constant strain amplitude can anneal it, relaxing a sample to a steady state that encodes a memory of that amplitude. This steady state also features a remarkable stability to amplitude variations that allows one to read the memory. Here we shed new light on both annealing and memory, by considering how to mechanically anneal a sample to have as little memory content as possible. In experiments, we show that a "ring-down" protocol reaches a comparable steady state, but with no discernible memories and minimal structural anisotropy…
The properties of the mixed system LiBH4 LiCl P2S5 are studied with respect to all-solid-state batteries. The studied material undergoes an amorphization upon heating above 601C, accompanied with increased Li+ conductivity beneficial for battery electrolyte applications. The measured ionic conductivity is 10-3 Scm-1 at room temperature with an activation energy of 0.40(2) eV after amorphization. Structural analysis and characterization of the material suggest that BH4 groups and PS4 may belong to the same molecular structure, where Cl ions interplay to accommodate the structural unit. Thanks t…
We use the general statement of the second law applied to an isolated system, the glass in an extremely large medium, to prove that the entropy of the glass must decrease with time during its relaxation towards the supercooled liquid state. This result contradicts the claim of Mauro et al and their computational result of the entropy, according to which their entropy of the glass increases. Our approach using the isolated system completely bypasses the issue of ergodicity loss in glasses, as discussed in the comment.
Recent scaling results for the AC conductivity of ionic glasses by Roling et al. [Phys. Rev. Lett. vol 78, 2160 (1997)] and Sidebottom [Phys. Rev. Lett. vol 82, 3653 (1999)] are discussed. It is shown that Sidebottom's version of scaling is completely general. A new analytical approximation to the universal AC conductivity of hopping in the extreme disorder limit, the ``diffusion cluster approximation,'' is presented and compared to simulations and experiments.
We determine the speed of a crystallisation (or more generally, a solidification) front as it advances into the uniform liquid phase after the system has been quenched into the crystalline region of the phase diagram. We calculate the front speed by assuming a dynamical density functional theory model for the system and applying a marginal stability criterion. Our results also apply to phase field crystal (PFC) models of solidification. As the solidification front advances into the unstable liquid phase, the density profile behind the advancing front develops density modulations and the wavele…
The effect of alternating shear orientation during cyclic loading on the relaxation dynamics in disordered solids is examined using molecular dynamics simulations. The model glass was initially prepared by rapid cooling from the liquid state and then subjected to cyclic shear along a single plane or periodically alternated in two or three dimensions. We showed that with increasing strain amplitude in the elastic range, the system is relocated to deeper energy minima. Remarkably, it was found that each additional alternation of the shear orientation in the deformation protocol brings the glass …
In crystals, molecules thermally vibrate around the periodic lattice sites. Vibrational motions are well understood in terms of phonons, which carry heat and control heat transport. The situation is notably different in disordered solids, where vibrational excitations are not phonons and can be even localized. Recent numerical work has established the concept of elastic heterogeneity: disordered solids show inhomogeneous local mechanical response. Clearly, the heterogeneous nature of elastic properties strongly influences vibrational and thermal properties, and it is expected to be the origin …
The relevant parameters at the microstructure scale that govern the macroscopic toughness of disordered brittle materials are investigated theoretically. We focus on planar crack propagation and describe the front evolution as the propagation of a long-range elastic line within a plane with random distribution of toughness. Our study reveals two regimes: in the collective pinning regime, the macroscopic toughness can be expressed as a function of a few parameters only, namely the average and the standard deviation of the local toughness distribution and the correlation lengths of the heterogen…
In the recent years, much attention has been devoted to the inhomogeneous nature of the mechanical response at the nano-scale in disordered solids. Clearly, the elastic heterogeneities that have been characterized in this context are expected to strongly impact the nature of the sound waves which, in contrast to the case of perfect crystals, cannot be completely rationalized in terms of phonons. Building on previous work on a toy model showing an amorphisation transition [Mizuno H, Mossa S, Barrat JL (2013) EPL {\bf 104}:56001], we investigate the relationship between sound waves and elastic h…
We comment on article by Yi Zhang , Hanna Terletska, Ka-Ming Tam, Yang Wang, Markus Eisenbach, Liviu Chioncel, and Mark Jarrell [Phys. Rev. B {\bf 100}, 054205 (2019)]\cite{Zhang} in which to study substitution disordered systems, they presented an embedding scheme for the locally self-consistent method. Here we show that their methods is a truncated case of our super-cell approximation, achieved by neglecting super-cell wave vectors dependence on self-energy $Σ_{sc}({\bf K}_{n},E)$ and replacing them by a local on-site self-energy, $Σ_{sc}({\bf K}_{n},E)=Σ_{sc}(L,L,E)$ in our articles\cite{Mo…
We report the first experimental demonstration of a TE-polarization photonic band gap (PBG) in a 2D isotropic hyperuniform disordered solid (HUDS) made of dielectric media with a index contrast of 1.6:1, very low for PBG formation. The solid is composed of a connected network of dielectric walls enclosing air-filled cells. Direct comparison with photonic crystals and quasicrystals permitted us to investigate band-gap properties as a function of increasing rotational isotropy. We present results from numerical simulations proving that the PBG observed experimentally for HUDS at low index contra…
Plastic yield of amorphous solids occurs by power law distributed slip avalanches whose universality is still debated. Determination of the power law exponents from experiments and molecular dynamics simulations is hampered by limited statistical sampling. On the other hand, while existing elasto-plastic depinning models give precise exponent values, these models to date have been limited to a scalar approximation of plasticity which is difficult to reconcile with the statistical isotropy of amorphous materials. Here we introduce for the first time a fully tensorial mesoscale model for the ela…
Supercells are often used in ab initio calculations to model compound alloys, surfaces and defects. One of the main challenges of supercell electronic structure calculations is to recover the Bloch character of electronic eigenstates perturbed by disorder. Here we apply the spectral weight approach to unfolding the electronic structure of group III-V and II-VI semiconductor solid solutions. The illustrative examples include: formation of donor-like states in dilute Ga(PN) and associated enhancement of its optical activity, direct observation of the valence band anticrossing in dilute GaAs:Bi, …
The influence of ordered regions (micro crystallites and aggregates) in the other wise disordered polymer host matrix on field and temperature dependence of mobility (μ) has been simulated. Increase in concentration of ordered regions leads to increase in magnitude of mobility and in high field regime the saturation of the mobility occurs at lower electric field strength. The influence of different mean and standard deviation of Gaussian density of states (DOS) of ordered regions on the field dependence of mobility was studied and found to be significant only at higher concentrations. Weak inf…
Viscoelasticity has been described since the time of Maxwell as an interpolation of purely viscous and purely elastic response, but its microscopic atomic-level mechanism in solids has remained elusive. We studied three model disordered solids: a random lattice, the bond-depleted fcc lattice, and the fcc lattice with vacancies. Within the harmonic approximation for central-force lattices, we applied sum-rules for viscoelastic response derived on the basis of non-affine atomic motions. The latter motions are a direct result of local structural disorder, and in particular, of the lack of inversi…
We show that the Fermi surface can survive the presence of extreme compositional disorder in the equiatomic alloy Ni$_{0.25}$Fe$_{0.25}$Co$_{0.25}$Cr$_{0.25}$. Our high-resolution Compton scattering experiments reveal a Fermi surface which is smeared across a significant fraction of the Brillouin zone (up to 40\% of $\frac{2π}{a}$). The extent of this smearing and its variation on and between different sheets of the Fermi surface has been determined, and estimates of the electron mean-free-path and residual resistivity have been made by connecting this smearing with the coherence length of the…
Understanding heat transport in semiconductors and insulators is of fundamental importance because of its technological impact in electronics and renewable energy harvesting and conversion. Anharmonic Lattice Dynamics provides a powerful framework for the description of heat transport at the nanoscale. One of the advantages of this method is that it naturally includes quantum effects due to atoms vibrations, which are needed to compute the thermal properties of semiconductors widely used in nanotechnology, like silicon and carbon, even at room temperature. While the heat transport picture subs…
Stress transmission in planar open-cell cellular solids is analysed using a recent theory developed for marginally rigid granular assemblies. This is made possible by constructing a one-to-one mapping between the two systems. General trivalent networks are mapped onto assemblies of rough grains, while networks where Plateau rules are observed, are mapped onto assemblies of smooth grains. The constitutive part of the stress transmission equations couples the stress directly to the local rotational disorder of the cellular structure via a new fabric tensor. An intriguing consequence of the analy…
To obtain the probability distribution of 2D crack patterns in mesoscopic regions of a disordered solid, the formalism of Paper I requires that a functional form associating the crack patterns (or states) to their formation energy be developed. The crack states are here defined by an order parameter field representing both the presence and orientation of cracks at each site on a discrete square network. The associated Hamiltonian represents the total work required to lead an uncracked mesovolume into that state as averaged over the initial quenched disorder. The effect of cracks is to create m…
Elastoplastic lattice models for the response of solids to deformation typically incorporate structure only implicitly via a local yield strain that is assigned to each site. However, the local yield strain can change in response to a nearby or even distant plastic event in the system. This interplay is key to understanding phenomena such as avalanches in which one plastic event can trigger another, leading to a cascade of events, but typically is neglected in elastoplastic models. To include the interplay one could calculate the local yield strain for a given particulate system and follow its…
This is the first of a series of three articles that treats fracture localization as a critical phenomenon. This first article establishes a statistical mechanics based on ensemble averages when fluctuations through time play no role in defining the ensemble. Ensembles are obtained by dividing a huge rock sample into many mesoscopic volumes. Because rocks are a disordered collection of grains in cohesive contact, we expect that once shear strain is applied and cracks begin to arrive in the system, the mesoscopic volumes will have a wide distribution of different crack states. These mesoscopic …
The time evolution and spatial correlations of nonaffine displacements in deformed amorphous solids are investigated using molecular dynamics simulations. The three-dimensional model glass is represented via the binary mixture, which is slowly annealed well below the glass transition temperature and then sheared at a constant strain rate. It is shown that with increasing strain, the typical size of clusters of atoms with large nonaffine displacements increases, and these clusters remain spatially homogeneously distributed, until the yielding point when mobile atoms become localized within a sy…
Molecular dynamics simulations with varying damping are used to examine the effects of inertia and spatial dimension on sheared disordered solids in the athermal, quasistatic limit. In all cases the distribution of avalanche sizes follows a power law over at least three orders of magnitude in dissipated energy or stress drop. Scaling exponents are determined using finite-size scaling for systems with thousands to millions of particles. Three distinct universality classes are identified corresponding to overdamped and underdamped limits, as well as a crossover damping that separates the two reg…
The interplay between the Fermi sea anisotropy, electron-electron interaction, and localization phenomena can give rise to exotic many-body phases. An exciting example is an anisotropic two-dimensional (2D) Wigner solid (WS), where electrons form an ordered array with an anisotropic lattice structure. Such a state has eluded experiments up to now as its realization is extremely demanding: First, a WS entails very low densities where the Coulomb interaction dominates over the kinetic (Fermi) energy. Attaining such low densities while keeping the disorder low is very challenging. Second, the low…
We investigate numerically and theoretically the precursory intermittent activity characterizing the preliminary phase of damage accumulation prior to failure of quasi-brittle solids. We use a minimal but thermodynamically consistent model of damage growth and localization developed by Berthier et al. (2017). The approach accounts for both microstructural disorder and non-local interactions and permits inferring a complete scaling description of the spatio-temporal structure of failure precursors. By developing a theoretical model of damage growth in disordered elasto-damageable specimen, we d…
