Recent theoretical studies of amorphous silicon [Y. Pan et al. Phys. Rev. Lett. 100 206403 (2008)] have revealed subtle but significant structural correlations in network topology: the tendency for short (long) bonds to be spatially correlated with other short (long) bonds). These structures were linked to the electronic band tails in the optical gap. In this paper, we further examine these issues for amorphous silicon, and demonstrate that analogous correlations exist in amorphous SiO2, and in the organic molecule, b-carotene. We conclude with a discussion of the origin of the effects and its possible generality.
The understanding of dynamic failure in amorphous materials via the propagation of free boundaries like cracks and voids must go beyond elasticity theory, since plasticity intervenes in a crucial and poorly understood manner near the moving free boundary. In this Letter we focus on failure via a cavitation instability in a radially-symmetric stressed material, set up the free boundary dynamics taking both elasticity and visco-plasticity into account, using the recently proposed athermal Shear Transformation Zone theory. We demonstrate the existence (in amorphous systems) of fast cavitation mod…
We have studied the statistics of plastic rearrangement events in a simulated amorphous solid at T=0. Events are characterized by the energy release and the ``slip volume'', the product of plastic strain and system volume. Their distributions for a given system size $L$ appear to be exponential, but a characteristic event size cannot be inferred, because the mean values of these quantities increase as $L^α$ with $α\sim 3/2$. In contrast to results obtained in 2D models, we do not see simply connected avalanches. The exponent suggests a fractal shape of the avalanches, which is also evidenced b…
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 derive a phase diagram for amorphous solids and liquid supercooled water and explain why the amorphous solids of water exist in several different forms. Application of large-deviation theory allows us to prepare such phases in computer simulations. Along with nonequilibrium transitions between the ergodic liquid and two distinct amorphous solids, we establish coexistence between these two amorphous solids. The phase diagram we predict includes a nonequilibrium triple point where two amorphous phases and the liquid coexist. While the amorphous solids are long-lived and slowly-aging glasses, …
Amorphous solids at low temperature display unusual features which have been escaped a clear and unified comprehension. In recent years a mean field theory of amorphous solids constructed in the limit of infinite spatial dimensions has been proposed. I will briefly review what is the outcome of this theory focusing the low temperature phase and discuss some perspectives to go beyond the mean field limit.
The low-frequency vibrational and low-temperature thermal properties of amorphous solids are markedly different from those of crystalline solids. This situation is counter-intuitive because any solid material is expected to behave as a homogeneous elastic body in the continuum limit, in which vibrational modes are phonons following the Debye law. A number of phenomenological explanations have been proposed, which assume elastic heterogeneities, soft localized vibrations, and so on. Recently, the microscopic mean-field theories have been developed to predict the universal non-Debye scaling law.…
We study excitations of atomic vibrations in the reciprocal space for amorphous solids. There are two kinds of excitations we obtained, collective excitation and local excitation. The collective excitation is the collective vibration of atoms in the amorphous solids while the local excitation is stimulated locally by a single atom vibrating in the solids. We introduce a continuous wave vector for the study and transform the equations of atomic vibrations from the real space to the reciprocal space. We take the amorphous silicon as an example and calculate the structures of the excitations in t…
We perform an extensive numerical study of avalanche behavior in a 2D LJ glass at T=0, sheared at finite strain rates $\dotγ$. From the finite size analysis of stress fluctuations and of transverse diffusion we show that flip-flip correlations remain relevant at all realistic strain rates. We predict that the avalanche size scales as $\dotγ^{-1/d}$, with $d$ the space dimension.
It is known by now that amorphous solids at zero temperature do not possess a nonlinear elasticity theory: besides the shear modulus which exists, all the higher order coefficients do not exist in the thermodynamic limit. Here we show that the same phenomenon persists up to temperatures comparable to the glass transition. The zero temperature mechanism due to the prevalence of dangerous plastic modes of the Hessian matrix is replaced by anomalous stress fluctuations that lead to the divergence of the variances of the higher order elastic coefficients. The conclusion is that in amorphous solids…
A different perspective on the long-standing problem of amorphous solidification is offered, based on an alternative definition of a solid as a porous medium. General, model-free results are obtained concerning the growing dynamic length accompanying solidification and its relation to the growing relaxation time. Criteria are derived for the dynamic length to diverge and for its divergence to entail the arrest of particle motion.
A number of current theories of plasticity in amorphous solids assume at their basis that plastic deformations are spatially localized. We present in this paper a series of numerical experiments to test the degree of locality of plastic deformation. These experiments increase in terms of the stringency of the removal of elastic contributions to the observed elasto-plastic deformations. It is concluded that for all our simulational protocols the plastic deformations are not localized, and their scaling is sub-extensive. We offer a number of measures of the magnitude of the plastic deformation, …
The question of the local stability of the (replica-symmetric) amorphous solid state is addressed for a class of systems undergoing a continuous liquid to amorphous-solid phase transition driven by the effect of random constraints. The Hessian matrix, associated with infinitesimal fluctuations around the stationary point corresponding to the amorphous solid state, is obtained. The eigenvalues of this Hessian matrix are all shown to be strictly positive near the transition, except for one--the zero mode associated with the spontaneously broken continuous translational symmetry of the system. Th…
Highly acurate numerical simulations are employed to highlight the subtle but important differences in the mechanical stability of perfect crystalline solids versus amorphous solids. We stress the difference between strain values at which the shear modulus vanishes and strain values at which a plastic instability insues. The temperature dependence of the yield strain is computed for the two types of solids, showing different scaling laws: $γ_{_{Y}}\simeq γ_{_{Y}}^{0}-C_1 T^{1/3}$ for crystals versus $γ_{_{Y}}\simeq γ_{_{Y}}^{0}- C_2 T^{2/3}$ for amorphous solids.
We study the statistical properties of the yielding transition in model amorphous solids in the limit of slow, athermal deformation. Plastic flow occurs via alternating phases of elastic loading punctuated by rapid dissipative events in the form of collective avalanches. We investigate their characterization through energy vs. stress drops and at multiple stages of deformation, thus revealing a change of spatial extent of the avalanches and degree of stress correlations as deformation progresses. We show that the statistics of stress and energy drops only become comparable for large events in …
The shear-modulus and yield-stress of amorphous solids are important material parameters, with the former determining the rate of increase of stress under external strain and the latter being the stress value at which the material flows in a plastic manner. It is therefore important to understand how these parameters can be related to the inter-particle potential. Here a scaling theory is presented such that given the inter-particle potential, the dependence of the yield stress and the shear modulus on the density of the solid can be predicted in the athermal limit. It is explained when such p…
We present a theoretical derivation of acoustic phonon damping in amorphous solids based on the nonaffine response formalism for the viscoelasticity of amorphous solids. The analytical theory takes into account the nonaffine displacements in transverse waves and is able to predict both the ubiquitous low-energy diffusive damping $\sim k^{2}$, as well as a novel contribution to the Rayleigh damping $\sim k^{4}$ at higher wavevectors and the crossover between the two regimes observed experimentally. The coefficient of the diffusive term is proportional to the microscopic viscous (Langevin-type) …
Amorphous solids increase their stress as a function of an applied strain until a mechanical yield point whereupon the stress cannot increase anymore, afterwards exhibiting a steady state with a constant mean stress. In stress controlled experiments the system simply breaks when pushed beyond this mean stress. The ubiquity of this phenomenon over a huge variety of amorphous solids calls for a generic theory that is free of microscopic details. Here we offer such a theory: the mechanical yield is a thermodynamic phase transition, where yield occurs as a spinodal phenomenon. At the spinodal poin…
We use atomistic computer simulations to provide a microscopic description of the brittle failure of amorphous materials, and we assess the role of rare events and quenched disorder. We argue that brittle yielding originates at rare soft regions, similarly to Griffiths effects in disordered systems. We numerically demonstrate how localized plastic events in such soft regions trigger macroscopic failure via the propagation of a shear band. This physical picture, which no longer holds in poorly annealed ductile materials, allows us to discuss the role of finite size effects in brittle yielding a…
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…
The distribution of local residual stresses (threshold to instability) that controls the statistical properties of plastic flow in athermal amorphous solids is examined with an atomistic simulation technique. For quiescent configurations, the distribution has a pseudogap (power-law) form with an exponent that agrees well with global yielding statistics. As soon as deformation sets in, the pseudogap region gives way to a system size dependent plateau at small residual stresses that can be understood from the statistics of local residual stress {\em differences} between plastic events. Results f…
We analyze the effect of temperature on the yielding transition of amorphous solids using different coarse-grained model approaches. On one hand we use an elasto-plastic model, with temperature introduced in the form of an Arrhenius activation law over energy barriers. On the other hand, we implement a Hamiltonian model with a relaxational dynamics, where temperature is introduced in the form of a Langevin stochastic force. In both cases, temperature transforms the sharp transition of the athermal case in a smooth crossover. We show that this thermally smoothed transition follows a simple scal…
Goldstone modes in the amorphous solid state, resulting from the spontaneous breaking of translational symmetry due to random localisation of particles, are discussed. Starting from a microscopic model with quenched disorder, the broken symmetry is identified to be that of relative translations of the replicas. Goldstone excitations, corresponding to pure shear deformations, are constructed from long wavelength distortions of the order parameter. The elastic free energy is computed, and it is shown that Goldstone fluctuations destroy localisation in two spatial dimensions, yielding a two-dimen…
Tunneling two-level systems (TLSs), generic to amorphous solids, dictate the low-temperature properties of amorphous solids and dominate noise and decoherence in quantum nano-devices. The properties of the TLSs are generally described by the phenomenological standard tunneling model. Yet, significant deviations from the predictions of this model found experimentally suggest the need for a more precise model in describing TLSs. Here we show that the temperature dependence of the sound velocity, dielectric constant, specific heat, and thermal conductivity, can be explained using an energy-depend…
We identify the possibility of realizing higher order topological (HOT) phases in noncrystalline or amorphous materials. Starting from two and three dimensional crystalline HOT insulators, accommodating topological corner states, we gradually enhance structural randomness in the system. Within a parameter regime, as long as amorphousness is confined by outer crystalline boundary, the system continues to host corner states, yielding amorphous HOT insulators. However, as structural disorder percolates to the edges, corner states start to dissolve into amorphous bulk, and ultimately the system be…
What characterises a solid is its way to respond to external stresses. Ordered solids, such crystals, display an elastic regime followed by a plastic one, both well understood microscopically in terms of lattice distortion and dislocations. For amorphous solids the situation is instead less clear, and the microscopic understanding of the response to deformation and stress is a very active research topic. Several studies have revealed that even in the elastic regime the response is very jerky at low temperature, resembling very much the one of disordered magnetic materials. Here we show that in…
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 …
In sufficiently high spatial dimensions, the formation of the amorphous (i.e. random) solid state of matter, e.g., upon sufficent crosslinking of a macromolecular fluid, involves particle localization and, concommitantly, the spontaneous breakdown of the (global, continuous) symmetry of translations. Correspondingly, the state supports Goldstone-type low energy, long wave-length fluctuations, the structure and implications of which are identified and explored from the perspective of an appropriate replica field theory. In terms of this replica perspective, the lost symmetry is that of relative…
Prestress in amorphous solids bears the memory of their formation, and plays a profound role in their mechanical properties, from stiffening or softening elastic moduli to shifting frequencies of vibrational modes, as well as directing yielding and solidification in the nonlinear regime. Here we develop a set of mathematical tools to investigate elasticity of prestressed discrete networks, which disentangles the effects from disorder in configuration and disorder in prestress. Applying these methods to prestressed triangular lattices and a computational model of amorphous solids, we demonstrat…
Plasticity in amorphous solids is mediated by localized quadrupolar instabilities, but the mechanism by which an amorphous solid eventually fails or melts is debated. In this work we argue that these phenomena can be investigated in the model problem of an elastic continuum with quadrupolar defects, at finite temperature. This problem is posed and the collective behavior of the defects is analytically investigated. Using both renormalization group and field-theoretic techniques, it is found that the model has a yielding/melting transition of spinodal type.
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.
The first two successful predictions for amorphous solid experiments by tunneling-two-level-system (TTLS) was phonon echo and saturation phenomena. In this paper by generalizing TTLS to infinite-level-system model with certain randomness and nonlinearity, we prove that phonon echo is a stimulated emission process. The classical infinite-level-system (taking $\hbar\to 0$ limit) cannot find saturation effect, while quantum infinite-level-system can find it with certain nonlinearity assumed. We also prove that without randomness or nonlinearity neither phonon echo nor saturation exists in arbitra…
Under sufficient permanent random covalent bonding, a fluid of atoms or small molecules is transformed into an amorphous solid network. Being amorphous, local structural properties in such networks vary across the sample. A natural order parameter, resulting from a statistical-mechanical approach, captures information concerning this heterogeneity via a certain joint probability distribution. This joint probability distribution describes the variations in the positional and orientational localization of the particles, reflecting the random environments experienced by them, as well as further i…
The motion of the structure determining components is highly collective, both in amorphous solids and in undercooled liquids. This has been deduced from experimental low temperature data in the tunneling regime as well as from the vanishing isotope effect in diffusion in glasses and undercooled liquids. In molecular dynamics simulations of glasses one observes that both low frequency resonant vibrations and atomic jumps are centered on more than 10 atoms which, in densely packed materials, form chainlike structures. With increasing temperature the number of atoms jumping collectively increases…
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…
We derive expressions for the shear modulus of deeply-quenched, glassy solids, in terms of a Cauchy-Born free energy expansion around a rigid (quenched) reference state, following the approach due to Alexander [Alexander, Phys. Rep. 296, 1998]. Continuum-limit explicit expressions of the shear modulus are derived starting from the microscopic Hamiltonians of central and bond-bending interactions. The applicability of the expressions to dense covalent glasses as well as colloidal glasses with strongly attractive and adhesive bonds is discussed.
We investigate the constraints on the superfluid fraction of an amorphous solid following from an upper bound derived by Leggett. In order to accomplish this, we use as input density profiles generated for amorphous solids in a variety of different manners including by investigating Gaussian fluctuations around classical results. These rough estimates suggest that, at least at the level of the upper bound, there is not much difference in terms of superfluidity between a glass and a crystal characterized by the same Lindemann ratio. Moreover, we perform Path Integral Monte Carlo simulations of …
We investigate the linear elastic response of amorphous solids to a shear strain at zero temperature. We find that the response is characterized by at least two distinct shear moduli. The first one, $μ_{\rm ZFC}$, is associated with the linear response of a single energy minimum. The second, $μ_{\rm FC}$, is related to sampling, through plastic events, an ensemble of distinct energy minima. We provide examples of protocols that allow one to measure both shear moduli. In agreement with a theoretical prediction based on the exact solution in infinite spatial dimensions, the ratio $μ_{\rm FC}/μ_{…
Amorphous solids are yield stress materials that flow when a sufficient load is applied. Their flow consists of periods of elastic loading interrupted by rapid stress drops, or avalanches, coming from microscopic rearrangements known as shear transformations (STs). Here we show that the spatial extent of avalanches in a steadily sheared amorphous solid has a profound effect on the distribution of local residual stresses $x$. We find that in this distribution, the most unstable sites are located in a system size dependent plateau. While the entrance into the plateau is set by the lower cutoff o…
Shanghai Jiao Tong University（上海交通大学）；Johns Hopkins University（约翰斯·霍普金斯大学）；University of Montpellier and CNRS（蒙彼利埃大学与法国国家科学研究中心）；Chengdu University of Technology（成都理工大学）
Low-temperature properties of crystalline solids can be understood using harmonic perturbations around a perfect lattice, as in Debye's theory. Low-temperature properties of amorphous solids, however, strongly depart from such descriptions, displaying enhanced transport, activated slow dynamics across energy barriers, excess vibrational modes with respect to Debye's theory (i.e., a Boson Peak), and complex irreversible responses to small mechanical deformations. These experimental observations indirectly suggest that the dynamics of amorphous solids becomes anomalous at low temperatures. Here,…
The damping or attenuation coefficient of sound waves in solids due to impurities scales with the wavevector to the fourth power, also known as Rayleigh scattering. In amorphous solids, Rayleigh scattering may be enhanced by a logarithmic factor although computer simulations offer conflicting conclusions regarding this enhancement and its microscopic origin. We present a tensorial replica field-theoretic derivation based on heterogeneous or fluctuating elasticity (HE), which shows that long-range (power-law) spatial correlations of the elastic constants, is the origin of the logarithmic enhanc…
We consider the effect of the internal nuclear quadrupole interaction on quantum tunneling in complex multi-atomic two-level systems. Two distinct regimes of strong and weak interactions are found. The regimes depend on the relationship between a characteristic energy of the nuclear quadrupole interaction $λ_{\ast}$ and a bare tunneling coupling strength $Δ_{0}$. When $Δ_{0}>λ_{\ast}$, the internal interaction is negligible and tunneling remains coherent determined by $Δ_{0}$. When $Δ_{0}<λ_{\ast}$, coherent tunneling breaks down and an effective tunneling amplitude decreases by an exponential…
The high frequency dynamics of low- (LDA) and high-density amorphous-ice (HDA) and of cubic ice (I_c) has been measured by inelastic X-ray Scattering (IXS) in the 1-15 nm^{-1} momentum transfer (Q) range. Sharp phonon-like excitations are observed, and the longitudinal acoustic branch is identified up to Q = 8nm^{-1} in LDA and I_c and up to 5nm^{-1} in HDA. The narrow width of these excitations is in sharp contrast with the broad features observed in all amorphous systems studied so far. The "crystal-like" behavior of amorphous ices, therefore, implies a considerable reduction in the number o…
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 …
