A link between structural ordering and slow dynamics has recently attracted much attention from the context of the origin of glassy slow dynamics. Candidates for such structural order are icosahedral, exotic amorphous and crystal-like. Each type of order is linked to a different scenario of glass transition. Here we experimentally access local structural order in polydisperse hard spheres by particle-level confocal microscopy. We identify the key structures as icosahedral and FCC-like order, both statistically associated with slow particles. However, when approaching the glass transition, the icosahedral order does not grow in size, whereas crystal-like order grows. It is the latter that governs the dynamics and is linked to dynamic heterogeneity. This questions the direct role of the local icosahedral ordering in glassy slow dynamics and suggests that the growing length scale of structural order is essential for the slowing down of dynamics and the non-local cooperativity in particle motion.
Biomaterials such as protein or polysaccharide gels are known to behave qualitatively as soft solids and to rupture under an external load. Combining optical and ultrasonic imaging to shear rheology we show that the failure scenario of a protein gel is reminiscent of brittle solids: after a primary creep regime characterized by a power-law behavior which exponent is fully accounted for by linear viscoelasticity, fractures nucleate and grow logarithmically perpendicularly to shear, up to the sudden rupture of the gel. A single equation accounting for those two successive processes nicely captures the full rheological response. The failure time follows a decreasing power law with the applied shear stress, similar to the Basquin law of fatigue for solids. These results are in excellent agreement with recent fiber-bundle models that include damage accumulation on elastic fibers and exemplify protein gels as model, brittle-like soft solids.PACS numbers: 82.35. Pq, 47.57.Qk, 83.80.Kn Biogels formed through the self-association of polysaccharide coils, collagen, actin filaments or attractive globular proteins play a major role in biochemistry and microbiology [1], biological networks and cell mechanics [2] as well as in food science [3]. These biomaterials all behave as elastic solids under small deformations but display remarkable nonlinear behavior generally featuring stress-or strain-stiffening [4] and fractures prior to irreversible rupture [5,6]. Irreversibility stems from the existence of an external control parameter, e.g. temperature or pH in the case of thermoreversible or acid-induced gels respectively. This makes such biogels fundamentally different from other soft glassy materials such as emulsions, colloidal gels and glasses that can be rejuvenated by shear [7][8][9][10] or transient networks where fractures spontaneously heal [11,12]. So far, huge effort has been devoted to the design of protein gels with specific properties and textures at rest [13,14]. However, their mechanical behavior deep into the nonlinear regime has only been partially addressed [15,16] and several fundamental issues remain unexplored such as the spatially resolved rupture scenario or the physical relevance of the analogy with brittle failure in hard solids.In this Letter we report on stress-induced fracture in protein gels by means of creep experiments coupled to optical and ultrasonic imaging. Gels formed by slow acidification of a sodium caseinate solution display fractures under large strain at fixed low pH values [15,17], which makes them perfect candidates to quantify the rupture of soft solids and tackle the above-mentioned issues. We demonstrate that under an external load, these casein gels display brittle-like failure that results from two successive physical processes: (i) a primary creep regime where dissipation is dominated by viscous flow through the gel matrix without any detectable macroscopic strain localization and (ii) the irreversible nucle-
Colloidal gels have unique mechanical and transport properties that stem from their bicontinuous nature, in which a colloidal network is intertwined with a viscous solvent, and have found numerous applications in foods, cosmetics, and construction materials and for medical applications, such as cartilage replacements. So far, our understanding of the process of colloidal gelation is limited to long-time dynamical effects, where gelation is viewed as a phase separation process interrupted by the glass transition. However, this purely out-of-equilibrium thermodynamic picture does not address the emergence of mechanical stability. With confocal microscopy experiments, we reveal that mechanical metastability is reached only after isotropic percolation of locally isostatic environments, establishing a direct link between the load-bearing ability of gels and the isostaticity condition. Our work suggests an operative description of gels based on mechanical equilibrium and isostaticity, providing the physical basis for the stability and rheology of these materials.
Most of the liquid-state theories, including glass-transition theories, are constructed on the basis of two-body density correlations. However, we have recently shown that many-body correlations, in particular, bond orientational correlations, play a key role in both the glass transition and the crystallization transition. Here we show, with numerical simulations of supercooled polydisperse hard spheres systems, that the length-scale associated with any two-point spatial correlation function does not increase toward the glass transition. A growing length-scale is instead revealed by considering many-body correlation functions, such as correlators of orientational order, which follows the length-scale of the dynamic heterogeneities. Despite the growing of crystal-like bond orientational order, we reveal that the stability against crystallization with increasing polydispersity is due to an increasing population of icosahedral arrangements of particles. Our results suggest that, for this type of systems, many-body correlations are a manifestation of the link between the vitrification and the crystallization phenomena. Whether a system is vitrified or crystallized can be controlled by the degree of frustration against crystallization, polydispersity in this case.
We study experimentally the response of a dense sediment of Brownian particles to self-propulsion. We observe that the ergodic supercooled liquid relaxation is monotonically enhanced by activity. By contrast the nonergodic glass shows an order of magnitude slowdown at low activities with respect to passive case, followed by fluidization at higher activities. Our results contrast with theoretical predictions of the ergodic approach to glass transition summing up to a shift of the glass line. We propose that nonmonotonicity is due to competing effects of activity: (i) extra energy that helps breaking cages (ii) directionality that hinders cage exploration. We call it "Deadlock from the Emergence of Active Directionality" (DEAD). It suggests further theoretical works should include thermal motion.A supercooled liquid is obtained when a system is cooled down, or compressed, beyond its freezing temperature while avoiding crystallization. This metastable state displays slow dynamics but remains ergodic. As the system is further cooled down or compressed, its dynamics slows down by orders of magnitude until the system becomes nonergodic, which means that it can explore only a small part of its potential energy landscape. It is an amorphous solid called a glass. Our understanding of this fundamental state of matter has tremendously progressed in the last decades [1,2]. Studying the glass transition under nonequilibrium conditions helps us define what are general properties of glassy systems and their emergent behaviors when they are driven out-of-equilibrium. This is where the field of active matter, which emerged as a new frontier of science, meets glassy physics. In the past years, the behavior of assemblies of self-propelled objects stepped up from a mere zoological curiosity to a flourishing field of nonequilibrium physics. Rather dilute assemblies of active particles have been studied extensively by experiments and numerical simulations [3][4][5][6][7][8][9]. Exploring the full range of densities including ordered phases has been done in some model systems [10-13] but dense amorphous systems remain largely unexplored experimentally. Dense assemblies of self-propelled particles sit at the convergence of active matter and glassy physics, and should constitute a test bed for other such systems as for example biological tissues [14,15].However, it is still unclear how self-propulsion would influence the glass transition. Numerical studies have found either activity-induced fluidization [16,17] or arrest [18,19]. It was found that the influence of activity could not be captured by a single parameter such as effective temperature, but that the persistence time of the propulsion direction played a major role and shifts the position of the glass transition line in nontrivial ways. For example in Ref.[20] glass transition shifts to higher densities with increasing persistence time at low effective temperature, whereas the opposite effect is observed at higher effective temperatures. Besides, Ref.[21] demonstrates that the mo...
We report the splitting of an oscillating DNA circuit into ∼700 droplets with picoliter volumes. Upon incubation at constant temperature, the droplets display sustained oscillations that can be observed for more than a day. Superimposed to the bulk behaviour, we find two intriguing new phenomena - slow desynchronization between the compartments and kinematic spatial waves - and investigate their possible origin. This approach provides a route to study the influence of small volume effects in biology, and paves the way to technological applications of compartmentalized molecular programs controlling complex dynamics.
Particle tracking is a key to single-particle-level confocal microscopy observation of colloidal suspensions, emulsions, and granular matter. The conventional tracking method has not been able to provide accurate information on the size of individual particle. Here we propose a novel method to localise spherical particles of arbitrary relative sizes from either 2D or 3D (confocal) images either in dilute or crowded environment. Moreover this method allows us to estimate the size of each particle reliably. We use this method to analyse local bond orientational ordering in a supercooled polydisperse colloidal suspension as well as the heterogeneous crystallisation induced by a substrate. For the former, we reveal non-trivial couplings of crystal-like bond orientational order and local icosahedral order with the spatial distribution of particle sizes: Crystal-like order tends to form in regions where very small particles are depleted and the slightly smaller size of the central particle stabilizes icosahedral order. For the latter, on the other hand, we found that very small particles are expelled from crystals and accumulated on the growth front of crystals. We emphasize that such information has not been accessible by conventional tracking methods. * mathieu.leocmach@polytechnique.org; Present address: Laboratoire de Physique,
We have developed a lab work module where we teach undergraduate students how to quantify the dynamics of a suspension of microscopic particles, measuring and analyzing the motion of those particles at the individual level or as a group. Differential Dynamic Microscopy (DDM) is a relatively recent technique that precisely does that and constitutes an alternative method to more classical techniques such as dynamics light scattering (DLS) or video particle tracking (VPT). DDM consists in imaging a particle dispersion with a standard light microscope and a camera. The image analysis requires the students to code and relies on digital Fourier transform to obtain the intermediate scattering function, an autocorrelation function that characterizes the dynamics of the dispersion. We first illustrate DDM on the textbook case of colloids where we measure the diffusion coefficient. Then we show that DDM is a pertinent tool to characterize biologic systems such as motile bacteria i.e.bacteria that can self propel, where we not only determine the diffusion coefficient but also the velocity and the fraction of motile bacteria. Finally, so that our paper can be used as a tutorial to the DDM technique, we have joined to this article movies of the colloidal and bacterial suspensions and the DDM algorithm in both Matlab and Python to analyze the movies.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.