Active systems, which are driven out of equilibrium by local non-conservative forces, can adopt unique behaviors and configurations. An important challenge in the design of novel materials which utilize such properties is to precisely connect the static structure of active systems to the dissipation of energy induced by the local driving. Here, we use tools from liquid-state theories and machine learning to take on this challenge. We first demonstrate analytically for an isotropic active matter system that dissipation and pair correlations are closely related when driving forces behave like an active temperature. We then extend a nonequilibrium mean-field framework for predicting these pair correlations, which unlike most existing approaches is applicable even for strongly interacting particles and far from equilibrium, to predicting dissipation in these systems. Based on this theory, we reveal a robust analytic relation between dissipation and structure which holds even as the system approaches a nonequilibrium phase transition. Finally, we construct a neural network which maps static configurations of particles to their dissipation rate without any prior knowledge of the underlying dynamics. Our results open novel perspectives on the interplay between dissipation and organization out-of-equilibrium.
We show that a generalized fluctuation-dissipation relation applies upon instantaneously increasing the temperature of a deeply supercooled liquid. This has the same two-step shape of the relation found upon cooling the liquid, but with opposite violation, indicating an effective temperature that is lower than bath temperature. We show that the effective temperature exhibits some sensible time-dependence and that it retains its connection with the partitioned phase space visited in ageing. We underline the potential relevance of our numerical results for experimental studies of the fluctuation…
The dynamics and structure of nonequilibrium liquids, driven by non-conservative forces which can be either external or internal, generically hold the signature of the net dissipation of energy in the thermostat. Yet, disentangling precisely how dissipation changes collective effects remains challenging in many-body systems due to the complex interplay between driving and particle interactions. First, we combine explicit coarse-graining and stochastic calculus to obtain simple relations between diffusion, density correlations and dissipation in nonequilibrium liquids. Based on these results, w…
We present evidence in favor of the possibility of treating an out-of-equilibrium supercooled simple liquid as a system in quasi-equilibrium. Two different temperatures, one controlled by the external bath and one internally selected by the system characterize the quasi-equilibrium state. The value of the internal temperature is explicitly calculated within the inherent structure thermodynamic formalism. We find that the internal temperature controls the relation between the response to an external perturbation and the long-time decay of fluctuations in the liquid.
Minimal models of active and driven particles have recently been used to elucidate many properties non-equilibrium systems. However, the relation between energy consumption and changes in the structure and transport properties of these non-equilibrium materials remains to be explored. We explore this relation in a minimal model of a driven liquid that settles into a time periodic steady state. Using concepts from stochastic thermodynamics and liquid state theories, we show how the work performed on the system by the various non-conservative, time dependent forces - this quantifies a violation …
Self-organization of active matter as well as driven granular matter in non-equilibrium dynamical states has attracted considerable attention not only from the fundamental and application viewpoints but also as a model to understand the occurrence of such phenomena in nature. These systems share common features originating from their intrinsically out-of-equilibrium nature. It remains elusive how energy dissipation affects the state selection in such non-equilibrium states. As a simple model system, we consider a non-equilibrium stationary state maintained by continuous energy input, relevant …
We report that the local Debye-Waller factor in a simulated 2D glass-forming mixture exhibits significant spatial heterogeneities and that these short time fluctuations provide an excellent predictor of the spatial distribution of the long time dynamic propensities [Phys.Rev.Lett. 93, 135701 (2004)]. In contrast, the potential energy per particle of the inherent structure does not correlate well with the spatially distributed dynamics.
We study the out-of-equilibrium dynamics following a temperature-jump in a model for a strong liquid, BKS-silica, and compare it with the well known case of fragile liquids. We calculate the fluctuation-dissipation relation, from which it is possible to estimate an effective temperature $T_{eff}$ associated to the slow out-of-equilibrium structural degrees of freedom. We find the striking and unexplained result that, differently from the fragile liquid cases, $T_{eff}$ is smaller than the bath temperature.
We explain the findings by Di Leonardo et al. [Phys. Rev. Lett. 84, 6054 (2000)] that the effective temperature of a Lennard-Jones glass depends only on the final value of the density in the volume and/or temperature jump that produces the glass phase. This is not only a property of the Lennard-Jones liquid, but a feature of all strongly correlating liquids. For such liquids data from a single quench simulation provides enough information to predict the effective temperature of any glass produced by jumping from an equilibrium state. This prediction is validated by simulations of the Kob-Ander…
We revisit the fundamental problem of liquid-liquid dewetting and perform a detailed comparison of theoretical predictions based on thin-film models with experimental measurements obtained by atomic force microscopy (AFM). Specifically, we consider the dewetting of a liquid polystyrene (PS) layer from a liquid polymethyl methacrylate (PMMA) layer, where the thicknesses and the viscosities of PS and PMMA layers are similar. The excellent agreement of experiment and theory reveals that dewetting rates for such systems follow no universal power law, in contrast to dewetting scenarios on solid sub…
Glass-to-glass and liquid-to-liquid phase transitions were observed many years ago in bulk and confined water with or without applied pressure. It is shown that they result from the competition of two-liquid phases separated by an enthalpy difference depending on temperature. The model is based on the classical nucleation equation of these phases completed by this enthalpy saving existing at all temperatures and a pressure contribution. The thermodynamic parameters of amorphous water, the multiple glass transition temperatures, the enthalpy changes, and the temperature of maximum density under…
The properties of nanoconfined fluids can be strikingly different from those of bulk liquids. A basic unanswered question is whether the equilibrium and dynamic consequences of confinement are related to each other in a simple way. We study this question by simulation of a liquid comprising asymmetric dumbbell-shaped molecules, which can be deeply supercooled without crystallizing. We find that the dimensionless structural relaxation times - spanning six decades as a function of temperature, density, and degree of confinement - collapse when plotted versus excess entropy. The data also collaps…
To most existing non-equilibrium theories, the modeling of non-isothermal processes was a hard task. Intrinsic difficulties involved the non-equilibrium temperature, the coexistence of conserved energy and dissipative entropy, etc. In this paper, by taking the non-isothermal flow of nematic liquid crystals as a typical example, we illustrated that thermodynamically consistent models in either vectorial or tensorial forms could be constructed within the framework of Conservation-Dissipation Formalism (CDF). And the classical isothermal Ericksen-Leslie model and Qian-Sheng model were shown to be…
We employ a free energy lattice Boltzmann method to study the dynamics of a ternary fluid system consisting of a liquid drop driven by a body force across a regularly textured substrate, infused by a lubricating liquid. We focus on the case of partial wetting lubricants and observe a rich interplay between contact line pinning and viscous dissipation at the lubricant ridge, which become dominant at large and small apparent angles respectively. Our numerical investigations further demonstrate that the relative importance of viscous dissipation at the lubricant ridge depends on the drop to lubri…
We investigate the self-assembly (crystallisation) of particles with hard cores and isotropic, square-well interactions, using a Monte Carlo scheme to simulate overdamped Langevin dynamics. We measure correlation and response functions during the early stages of assembly, and we analyse the results using fluctuation-dissipation theorems, aiming to predict which systems will self-assemble successfully and which will get stuck in disordered states. The early-time correlation and response measurements are made before significant crystallisation has taken place, indicating that dynamical measureme…
Soft-elasticity in monodomain liquid crystal elastomers (LCEs) is promising for impact-absorbing applications where strain energy is ideally absorbed at constant stress. Conventionally, compressive and impact studies on LCEs have not been performed given the notorious difficulty synthesizing sufficiently large monodomain devices. Here we demonstrate 3D printing bulk ($>cm^3$) monodomain LCE devices using direct ink writing and study their compressive soft-elasticity over 8 decades of strain rate. At quasi-static rates, the monodomain soft-elastic LCE dissipated 45% of strain energy while compa…
When sand flows out of a funnel onto a surface, a three dimensional pile that is stabilized by friction grows taller as it spreads. Here we investigate an idealized two dimensional analogue: spreading of a pile of monodisperse oil droplets at a boundary. In our system the droplets are buoyant, adhesive, and in contrast to sand, here friction is negligible. The buoyant droplets are added to the pile one-at-a-time. As the aggregate grows, it reaches a critical height and the 2D pile spreads out across the barrier. We find that, while granularity is important, the growth process is reminiscent of…
A thorough understanding of the energy dissipation in the dynamics of wet granular matter is essential for a continuum description of natural phenomena such as debris flow, and the development of various industrial applications such as the granulation process. The coefficient of restitution (COR), defined as the ratio between the relative rebound and impact velocities of a binary impact, is frequently used to characterize the amount of energy dissipation associated. We measure the COR by tracing a freely falling sphere bouncing on a wet surface with the liquid film thickness monitored opticall…
Soft materials including elastomers and gels are pervasive in biological systems and technological applications. Whereas it is known that intrinsic fracture energies of soft materials are relatively low, how the intrinsic fracture energy cooperates with mechanical dissipation in process zone to give high fracture toughness of soft materials is not well understood. In addition, it is still challenging to predict fracture energies and crack-tip strain fields of soft tough materials. Here, we report a scaling theory that accounts for synergistic effects of intrinsic fracture energies and dissipat…
Viscosity ($η$) is one of the most important properties of disordered matter. The temperature-dependence of viscosity is used to adjust process variables for glass-making, from melting to annealing. The aim of this work was to develop a physics-informed machine learning model capable of predicting $η(T)$ of oxide liquids. Instead of predicting the viscosity itself, the NN predicts the parameters of the MYEGA viscosity equation: the liquid's fragility index, the glass transition temperature, and the asymptotic viscosity. With these parameters, $η$ can be computed at any temperature of interest,…
Molecular dynamics simulations have been performed to study frictional slip and its influence on energy dissipation and momentum transfer at atomically smooth solid/water interfaces. By modifying surface chemistry, we investigate the relationship between slip and the mechanical response of a vibrating solid for both hydrophilic and hydrophobic surfaces. We discover physical phenomena that emerge at high frequencies and that have significant contributions to energy dissipation. A new analytical model is developed to describe mechanical response of the resonators in this high frequency regime, w…
We investigate freely expanding sheets formed by ultrasoft gel beads, and liquid and viscoelastic drops, produced by the impact of the bead or drop on a silicon wafer covered with a thin layer of liquid nitrogen that suppresses viscous dissipation thanks to an inverse Leidenfrost effect. Our experiments show a unified behaviour for the impact dynamics that holds for solids, liquids, and viscoelastic fluids and that we rationalize by properly taking into account elastocapillary effects. In this framework, the classical impact dynamics of solids and liquids as far as viscous dissipation is negli…
The research herein studies the Langevin dynamics allowing for an exchange of energy between liquid crystals and the thermal environment. This dynamics leads to fluctuation and dissipation behaviors in the motions of liquid crystals, and therefore drives the system toward non-equilibrium evolutional processes. In particular, for the operations of liquid-crystal metastable systems, the fluctuation could allow an excitation (non-equilibrium) transition against energy barriers to the globally-stable state. Implemented with an actual case of liquid crystal pi configuration, this work statistically…
Based on a recently introduced analytical strategy [Hollingshead et al., J. Chem. Phys. 139, 161102 (2013)], we present a web applet that can quickly and semi-quantitatively estimate the equilibrium radial distribution function and related thermodynamic properties of a fluid from knowledge of its pair interaction. We present a detailed description of the applet's features and intended workflow, followed by a description of how the applet can be used to illustrate two (of many possible) concepts of interest for introductory statistical mechanics courses: the transition from ideal gas-like behav…
Time-dependent dynamical properties of a fluid can not be estimated from a single configuration without performing a simulation. Here we show, however, that the scaling properties of both structure and dynamics can be predicted from a single configuration. The new method is demonstrated to work very well for equilibrium dynamics of the Kob-Andersen Binary Lennard-Jones mixture. Furthermore, the method is applied to isobaric cooling where the liquid falls out of equilibrium and forms a glass, demonstrating that the method requires neither equilibrium nor constant volume conditions to work, in c…
Direct observation of vortex liquid droplets in the iron pnictide superconductor CaKAs$_4$Fe$_4$ at $0.5T$_c$
Universidad Autónoma de Madrid（马德里自治大学）；Michigan State University（密歇根州立大学）；Ames National Laboratory, Iowa State University（爱荷华州立大学艾姆斯国家实验室）；Iowa State University（爱荷华州立大学）；Universidad de Buenos Aires（布宜诺斯艾利斯大学）
