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Register a new userIsomorph theory of physical aging
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Jeppe C. Dyre
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This paper derives and discusses the configuration-space Langevin equation describing a physically aging R-simple system and the corresponding Smoluchowski equation. Externally controlled thermodynamic variables like temperature, density, pressure enter the description via the single parameter ${T}_{rm s}/T$ in which $T$ is the bath temperature and ${T}_{rm s}$ is the systemic temperature defined at any time $t$ as the thermodynamic equilibrium temperature of the state point with density $rho(t)$ and potential energy $U(t)$. In equilibrium ${T}_{rm s}cong T$ with fluctuations that vanish in the thermodynamic limit. In contrast to Tools fictive temperature and other effective temperatures in glass science, the systemic temperature is defined for any configuration with a well-defined density, even if it is not in any sense close to equilibrium. Density and systemic temperature define an aging phase diagram in which the aging system traces out a curve. Predictions are discussed for aging following various density-temperature and pressure-temperature jumps from one equilibrium state to another, as well as for a few other scenarios. The proposed theory implies that R-simple glass-forming liquids are characterized by a dynamic Prigogine-Defay ratio of unity.
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This paper generalizes isomorph theory to systems that are not in thermal equilibrium. The systems are assumed to be R-simple, i.e., have a potential energy that as a function of all particle coordinates $textbf{R}$ obeys the hidden-scale-invariance condition $U(textbf{R}_{rm a})<U(textbf{R}_{rm b})Rightarrow U(lambdatextbf{R}_{rm a})<U(lambdatextbf{R}_{rm b})$. Systemic isomorphs are introduced as lines of constant excess entropy in the phase diagram defined by density and systemic temperature, which is the temperature of the equilibrium state point with average potential energy equal to $U(textbf{R})$. The dynamics is invariant along a systemic isomorph if there is a constant ratio between the systemic and the bath temperature. In thermal equilibrium, the systemic temperature is equal to the bath temperature and the original isomorph formalism is recovered. The new approach rationalizes within a consistent framework previously published observations of isomorph invariance in simulations involving nonlinear steady-state shear flows, zero-temperature plastic flows, and glass-state isomorphs. The paper relates briefly to granular media, physical aging, and active matter. Finally, we discuss the possibility that the energy unit defining reduced quantities should be based on the systemic rather than the bath temperature.
Many experiments show that protein condensates formed by liquid-liquid phase separation exhibit aging rheological properties. Quantitatively, recent experiments by Jawerth et al. (Science 370, 1317, 2020) show that protein condensates behave as aging Maxwell fluids with an increasing relaxation time as the condensates age. Despite the universality of this aging phenomenon, a theoretical understanding of this aging behavior is lacking. In this work, we propose a mesoscopic model of protein condensates in which a phase transition from aging phase to non-aging phase occurs as the control parameter changes, such as temperature. The model predicts that protein condensates behave as viscoelastic Maxwell fluids at all ages, with the macroscopic viscosity increasing over time. The model also predicts that protein condensates are non-Newtonian fluids under a constant shear rate with the shear stress increasing over time. Our model successfully explains multiple existing experimental observations and also makes general predictions that are experimentally testable.
Recent experiments and simulations have revealed glassy features in the cytoplasm, living tissues as well as dense assemblies of self propelled colloids. This leads to a fundamental question: how do these non-equilibrium (active) amorphous materials differ from conventional passive glasses, created either by lowering temperature or by increasing density? To address this we investigate the aging behaviour after a quench to an almost arrested state of a model active glass former, a Kob-Andersen glass in two dimensions. Each constituent particle is driven by a constant propulsion force whose direction diffuses over time. Using extensive molecular dynamics simulations we reveal rich aging behaviour of this dense active matter system: short persistence times of the active forcing lead to effective thermal aging; in the opposite limit we find a two-step aging process with active athermal aging at short times followed by activity-driven aging at late times. We develop a dedicated simulation method that gives access to this long-time scaling regime for highly persistent active forces.
The far-from-equilibrium dynamics of glassy systems share important phenomenological traits. A transition is generally observed from a time-homogeneous dynamical regime to an aging regime where physical changes occur intermittently and, on average, at a decreasing rate. It has been suggested that a global change of the independent time variable to its logarithm may render the aging dynamics homogeneous: for colloids, this entails diffusion but on a logarithmic time scale. Our novel analysis of experimental colloid data confirms that the mean square displacement grows linearly in time at low densities and shows that it grows linearly in the logarithm of time at high densities. Correspondingly, pairs of particles initially in close contact survive as pairs with a probability which decays exponentially in either time or its logarithm. The form of the Probability Density Function of the displacements shows that long-ranged spatial correlations are very long-lived in dense colloids. A phenomenological stochastic model is then introduced which relies on the growth and collapse of strongly correlated clusters (dynamic heterogeneity), and which reproduces the full spectrum of observed colloidal behaviors depending on the form assumed for the probability that a cluster collapses during a Monte Carlo update. In the limit where large clusters dominate, the collapse rate is ~1/t, implying a homogeneous, log-Poissonian process that qualitatively reproduces the experimental results for dense colloids. Finally an analytical toy-model is discussed to elucidate the strong dependence of the simulation results on the integrability (or lack thereof) of the cluster collapse probability function.
Colloidal dispersions of Laponite platelets are known to age slowly from viscous sols to colloidal glasses. We follow this aging process by monitoring the diffusion of probe particles embedded in the sample via dynamic light scattering. Our results show that the time-dependent diffusion of the probe particles scales with their size. This implies that the fluctuation-dissipation theorem can be generalized for this out-of-equilibrium system by replacing the bath temperature with an effective temperature. Simultaneous dynamic rheological measurements reveal that this effective temperature increases as a function of aging time and frequency. This suggests the existence of two regimes: at probed time scales longer than the characteristic relaxation time of the Laponite dispersion, the system thermalizes with the bath, whereas at shorter time scales, the system is out-of-equilibrium with an effective temperature greater than the bath temperature.
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