arXiv subjects

J. S. Langer

Publications and source records attributed to J. S. Langer.

At least 37 records · Page 2Linked to original sources

arXiv2012

Ising Model of the Glassy Correlation Length

Recent numerical simulations indicate that several different equilibrium glass transitions may be characterized by diverging correlation lengths, and that these divergences are described by a non-mean-field, Ising-like, critical exponent. I argue here that a minimal model of polydisperse, hard-core particles can be reformulated in terms of Ising spins. The two spin states correspond, at high pressure, to two compact, local topologies -- "solidlike" and "liquidlike" -- whose average volumes per particle are nearly identical for strongly frustrated, glass forming systems. The critical correlations in this system imply a Vogel-Fulcher-Tamann formula for the structural relaxation time. The theory also predicts, however, that realistic glass-forming systems generally are not exactly critical and, therefore, do not exhibit ideal glass transitions at low temperatures or high pressures.

cond-mat.stat-mech↗

arXiv2012

Glass Dynamics at High Strain Rates

We present a shear-transformation-zone (STZ) theoretical analysis of molecular-dynamics simulations of a rapidly sheared metallic glass. These simulations are especially revealing because, although they are limited to high strain rates, they span temperatures ranging from well below to well above the glass transition. With one important discrepancy, the STZ theory reproduces the simulation data, including the way in which those data can be made to collapse onto simple curves by a scaling transformation. The STZ analysis implies that the system's behavior at high strain rates is controlled primarily by effective-temperature thermodynamics, as opposed to system-specific details of the molecular interactions. The discrepancy between theory and simulations occurs at the lower strain rates for temperatures near the glass transition. We argue that this discrepancy can be resolved by the same multi-species generalization of STZ theory that has been proposed recently for understanding frequency-dependent viscoelastic responses, Stokes-Einstein violations, and stretched-exponential relaxation in equilibrated glassy materials.

cond-mat.mtrl-sci↗

arXiv2012

Non-equilibrium thermodynamics in sheared hard-sphere materials

We combine the shear-transformation-zone (STZ) theory of amorphous plasticity with Edwards' statistical theory of granular materials to describe shear flow in a disordered system of thermalized hard spheres. The equations of motion for this system are developed within a statistical thermodynamic framework analogous to that which has been used in the analysis of molecular glasses. For hard spheres, the system volume $V$ replaces the internal energy $U$ as a function of entropy $S$ in conventional statistical mechanics. In place of the effective temperature, the compactivity $X = \partial V / \partial S$ characterizes the internal state of disorder. We derive the STZ equations of motion for a granular material accordingly, and predict the strain rate as a function of the ratio of the shear stress to the pressure for different values of a dimensionless, temperature-like variable near a jamming transition. We use a simplified version of our theory to interpret numerical simulations by Haxton, Schmiedeberg and Liu, and in this way are able to obtain useful insights about internal rate factors and relations between jamming and glass transitions.

cond-mat.stat-mech↗

arXiv2012

Shear-Transformation-Zone Theory of Viscosity, Diffusion, and Stretched Exponential Relaxation in Amorphous Solids

The shear-transformation-zone (STZ) theory has been remarkably successful in accounting for broadly peaked, frequency-dependent, viscoelastic responses of amorphous systems near their glass temperatures $T_g$. This success is based on the theory's first-principles prediction of a wide range of internal STZ transition rates. Here, I show that the STZ rate-distribution causes the Newtonian viscosity to be strongly temperature dependent; and I propose that it is this temperature dependence, rather than any heterogeneity-induced enhancement of diffusion, that is responsible for Stokes-Einstein violations near $T_g$. I also show that stretched-exponential relaxation of density fluctuations emerges naturally from the same distribution of STZ transition rates that predicts the viscoelastic behavior. To be consistent with observations of Fickian diffusion near $T_g$, however, an STZ-based diffusion theory somehow must include the cascades of correlated displacement events that are seen in low-temperature numerical simulations.

cond-mat.stat-mech↗

arXiv2011

Shear-Transformation-Zone Theory of Glassy Diffusion, Stretched Exponentials, and the Stokes-Einstein Relation

The success of the shear-transformation-zone (STZ) theory in accounting for broadly peaked, frequency-dependent, glassy viscoelastic response functions is based on the theory's first-principles prediction of a wide range of internal STZ transition rates. Here, I propose that the STZ's are the dynamic heterogeneities frequently invoked to explain Stokes-Einstein violations and stretched-exponential relaxation in glass-forming materials. I find that, to be consistent with observations of Fickian diffusion near $T_g$, an STZ-based diffusion theory must include cascades of correlated events, but that the temperature dependence of the Stokes-Einstein ratio is determined by an STZ-induced enhancement of the viscosity. Stretched-exponential relaxation of density fluctuations emerges from the same distribution of STZ transition rates that predicts the viscoelastic behavior.

cond-mat.stat-mech↗

arXiv2011

Shear-Transformation-Zone Theory of Linear Glassy Dynamics

We present a linearized shear-transformation-zone (STZ) theory of glassy dynamics in which the internal STZ transition rates are characterized by a broad distribution of activation barriers. For slowly aging or fully aged systems, the main features of the barrier-height distribution are determined by the effective temperature and other near-equilibrium properties of the configurational degrees of freedom. Our theory accounts for the wide range of relaxation rates observed in both structural glasses and soft glassy materials such as colloidal suspensions. We find that the frequency dependent loss modulus is not just a superposition of Maxwell modes. Rather, it exhibits an $α$ peak that rises near the viscous relaxation rate and, for nearly jammed, glassy systems, extends to much higher frequencies in accord with experimental observations. We also use this theory to compute strain recovery following a period of large, persistent deformation and then abrupt unloading. We find that strain recovery is determined in part by the initial barrier-height distribution, but that true structural aging also occurs during this process and determines the system's response to subsequent perturbations. In particular, we find by comparison with experimental data that the initial deformation produces a highly disordered state with a large population of low activation barriers, and that this state relaxes quickly toward one in which the distribution is dominated by the high barriers predicted by the near-equilibrium analysis. The nonequilibrium dynamics of the barrier-height distribution is the most important of the issues raised and left unresolved in this paper.

cond-mat.mtrl-sci↗

arXiv2011

Linear Response Theory for Hard and Soft Glassy Materials

Despite qualitative differences in their underlying physics, both hard and soft glassy materials exhibit almost identical linear rheological behaviors. We show that these nearly universal properties emerge naturally in a shear-transformation-zone (STZ) theory of amorphous plasticity, extended to include a broad distribution of internal thermal-activation barriers. The principal features of this barrier distribution are predicted by nonequilibrium, effective-temperature thermodynamics. Our theoretical loss modulus $G"(ω)$ has a peak at the $α$ relaxation rate, and a power law decay of the form $ω^{-ζ}$ for higher frequencies, in quantitative agreement with experimental data.

cond-mat.mtrl-sci↗

arXiv2010

Scientific interview

Four leading scientists in the field of the glass transition answer to a series of questions formulated by the Editors (L. Berthier, G. Biroli, J.-P. Bouchaud, L. Cipelletti, W. van Saarloos). No specific format has been imposed to their answers: the scientists were free to answer or not to any given question, using how much space they felt appropriate. After a first round of answers, each author was given the opportunity to read the answers by his colleagues and to adjust his own answers accordingly.

cond-mat.stat-mech↗

arXiv2010

Thermodynamic theory of dislocation-mediated plasticity

We reformulate the theory of polycrystalline plasticity, in externally driven, nonequilibrium situations, by writing equations of motion for the flow of energy and entropy associated with dislocations. Within this general framework, and using a minimal model of thermally assisted depinning with essentially only one adjustable parameter, we find that our theory fits the strain-hardening data for Cu over a wide range of temperatures and six decades of strain rate. We predict the transition between stage II and stage III hardening, including the observation that this transition occurs at smaller strains for higher temperatures. We also explain why strain-rate hardening is very weak up to large rates; and, with just one additional number, we accurately predict the crossover to power-law rate hardening in the strong-shock regime. Our analysis differs in several important respects from conventional dislocation-mediated continuum theories. We provide some historical background and discuss our rationale for these differences.

cond-mat.mtrl-sci↗

arXiv2010

Nonequilibrium Thermodynamics of the Kovacs Effect

We present a thermodynamic theory of the Kovacs effect based on the idea that the configurational degrees of freedom of a glass-forming material are driven out of equilibrium with the heat bath by irreversible thermal contraction and expansion. We assume that the slowly varying configurational subsystem, i.e. the part of the system that is described by inherent structures, is characterized by an effective temperature, and contains a volume-related internal variable. We examine mechanisms by which irreversible dynamics of the fast, kinetic-vibrational degrees of freedom can cause the entropy and the effective temperature of the configurational subsystem to increase during sufficiently rapid changes in the bath temperature. We then use this theory to interpret the numerical simulations by Mossa and Sciortino (MS), who observe the Kovacs effect in more detail than is feasible in laboratory experiments. Our analysis highlights two mechanisms for the equilibration of internal variables. In one of these, an internal variable first relaxes toward a state of quasi-equilibrium determined by the effective temperature, and then approaches true thermodynamic equilibrium as the effective temperature slowly relaxes toward the bath temperature. In the other mechanism, an internal variable directly equilibrates with the bath temperature on intermediate timescales, without equilibrating with the effective temperature at any stage. Both mechanisms appear to be essential for understanding the MS results.

cond-mat.mtrl-sci↗

arXiv2009

Nonequilibrium Thermodynamics of Amorphous Materials I: Internal Degrees of Freedom and Volume Deformation

This is the first of three papers devoted to the nonequilibrium thermodynamics of amorphous materials. Our focus here is on the role of internal degrees of freedom in determining the dynamics of such systems. For illustrative purposes, we study a solid whose internal degrees of freedom are vacancies that govern irreversible volume changes. Using this model, we compare a thermodynamic theory based on the Clausius-Duhem inequality to a statistical analysis based directly on the law of increase of entropy. The statistical theory is used first to derive the the Clausius-Duhem inequality. We then use the theory to go beyond those results and obtain detailed equations of motion, including a rate factor that is enhanced by deformation-induced noisy fluctuations. The statistical analysis points to the need for understanding how both energy and entropy are shared by the vacancies and their environments.

cond-mat.mtrl-sci↗

arXiv2009

Nonequilibrium Thermodynamics of Amorphous Materials II: Effective-Temperature Theory

We develop a theory of the effective disorder temperature in glass-forming materials driven away from thermodynamic equilibrium by external forces. Our basic premise is that the slow configurational degrees of freedom of such materials are weakly coupled to the fast kinetic/vibrational degrees of freedom, and therefore that these two subsystems can be described by different temperatures during deformation. We use results from the preceding paper on the nonequilibrium thermodynamics of systems with internal degrees of freedom to derive an equation of motion for the effective temperature and to learn how this temperature couples to the dynamics of the system as a whole.

cond-mat.mtrl-sci↗

arXiv2009

Nonequilibrium Thermodynamics of Amorphous Materials III: Shear-Transformation-Zone Plasticity

We use the internal-variable, effective-temperature thermodynamics developed in two preceding papers to reformulate the shear-transformation-zone (STZ) theory of amorphous plasticity. As required by the preceding analysis, we make explicit approximations for the energy and entropy of the STZ internal degrees of freedom. We then show that the second law of thermodynamics constrains the STZ transition rates to have an Eyring form as a function of the effective temperature. Finally, we derive an equation of motion for the effective temperature for the case of STZ dynamics.

cond-mat.mtrl-sci↗

arXiv2008

Rate dependent shear bands in a shear transformation zone model of amorphous solids

We use Shear Transformation Zone (STZ) theory to develop a deformation map for amorphous solids as a function of the imposed shear rate and initial material preparation. The STZ formulation incorporates recent simulation results [Haxton and Liu, PRL 99 195701 (2007)] showing that the steady state effective temperature is rate dependent. The resulting model predicts a wide range of deformation behavior as a function of the initial conditions, including homogeneous deformation, broad shear bands, extremely thin shear bands, and the onset of material failure. In particular, the STZ model predicts homogeneous deformation for shorter quench times and lower strain rates, and inhomogeneous deformation for longer quench times and higher strain rates. The location of the transition between homogeneous and inhomogeneous flow on the deformation map is determined in part by the steady state effective temperature, which is likely material dependent. This model also suggests that material failure occurs due to a runaway feedback between shear heating and the local disorder, and provides an explanation for the thickness of shear bands near the onset of material failure. We find that this model, which resolves dynamics within a sheared material interface, predicts that the stress weakens with strain much more rapidly than a similar model which uses a single state variable to specify internal dynamics on the interface.

cond-mat.soft↗

arXiv2008

Anomalous diffusion in heterogeneous glass-forming liquids: Temperature-dependent behavior

In a preceding paper, Mukhopadhyay and I studied the diffusive motion of a tagged molecule in a heterogeneous glass-forming liquid at temperatures just above a glass transition. Among other features of this system, we postulated a relation between heterogeneity and stretched-exponential decay of correlations, and we also confirmed that systems of this kind generally exhibit non-Gaussian diffusion on intermediate length and time scales. Here I extend this analysis to higher temperatures approaching the point where the heterogeneities disappear and thermal activation barriers become small. I start by modifying the continuous-time random-walk theory proposed earlier, and supplement this analysis with an extension of the excitation-chain theory of glass dynamics. I also use a key result from the shear-transformation-zone theory of viscous deformation of amorphous materials. Elements of each of these theories are then used to interpret experimental data for ortho-terphenyl, specifially, the diffusion and viscosity coefficients and neutron scattering measurements of the self intermediate scattering function. Reconciling the theory with these data sets provides insights about the crossover between super-Arrhenius and Arrhenius dynamics, length scales of spatial heterogeneities, violation of the Stokes-Einstein relation in glass-forming liquids, and the origin of stretched exponential decay of correlations.

cond-mat.stat-mech↗

arXiv2008

Anomalous diffusion and stretched exponentials in heterogeneous glass-forming liquids: Low-temperature behavior

We propose a model of a heterogeneous glass forming liquid and compute the low-temperature behavior of a tagged molecule moving within it. This model exhibits stretched-exponential decay of the wavenumber-dependent, self intermediate scattering function in the limit of long times. At temperatures close to the glass transition, where the heterogeneities are much larger in extent than the molecular spacing, the time dependence of the scattering function crosses over from stretched-exponential decay with an index $b=1/2$ at large wave numbers to normal, diffusive behavior with $b = 1$ at small wavenumbers. There is a clear separation between early-stage, cage-breaking $β$ relaxation and late-stage $α$ relaxation. The spatial representation of the scattering function exhibits an anomalously broad exponential (non-Gaussian) tail for sufficiently large values of the molecular displacement at all finite times.

cond-mat.mtrl-sci↗

arXiv2007

Shear-transformation-zone theory of plastic deformation near the glass transition

The shear-transformation-zone (STZ) theory of plastic deformation in glass-forming materials is reformulated in light of recent progress in understanding the roles played the effective disorder temperature and entropy flow in nonequilibrium situations. A distinction between fast and slow internal state variables reduces the theory to just two coupled equations of motion, one describing the plastic response to applied stresses, and the other the dynamics of the effective temperature. The analysis leading to these equations contains, as a byproduct, a fundamental reinterpretation of the dynamic yield stress in amorphous materials. In order to put all these concepts together in a realistic context, the paper concludes with a reexamination of the experimentally observed rheological behavior of a bulk metallic glass. That reexamination serves as a test of the STZ dynamics, confirming that system parameters obtained from steady-state properties such as the viscosity can be used to predict transient behaviors.

cond-mat.mtrl-sci↗

arXiv2007

Steady-state, effective-temperature dynamics in a glassy material

We present an STZ-based analysis of numerical simulations by Haxton and Liu (HL). The extensive HL data sharply test the basic assumptions of the STZ theory, especially the central role played by the effective disorder temperature as a dynamical state variable. We find that the theory survives these tests, and that the HL data provide important and interesting constraints on some of its specific ingredients. Our most surprising conclusion is that, when driven at various constant shear rates in the low-temperature glassy state, the HL system exhibits a classic glass transition, including super-Arrhenius behavior, as a function of the effective temperature.

cond-mat.soft↗