The dynamics of binary colloidal mixture subjected to an external potential barrier is investigated using molecular dynamics simulations. The depletion interactions between the potential barrier and larger components of the mixture alters the dynamics of the system significantly. The larger particles undergo sub-Arrhenius diffusion while smaller particles obey normal Arrhenius diffusion. These results show that quantum phenomena such as tunneling is not required to have sub-Arrhenius diffusion, in contrast to the general agreement in the literature. The depletion interactions between the external potential barrier and larger component increases with decreasing temperature which makes the effective activation energy for barrier crossing temperature dependent leading to sub-Arrhenius diffusion.
We report results from the molecular dynamics simulations of a binary colloidal mixture subjected to an external potential barrier along one of the spatial directions at low volume fraction, ϕ = 0.2. The variations in the asymmetry of the external potential barrier do not change the dynamics of the smaller particles, showing Arrhenius diffusion. However, the dynamics of the larger particles shows a crossover from sub-Arrhenius to super-Arrhenius diffusion with the asymmetry in the external potential at the low temperatures and low volume fraction. Super-Arrhenius diffusion is generally observe…
A binary colloidal mixture of unequal sizes, subjected to an external potential barrier, has been investigated using canonical ensemble molecular dynamics simulations. The attractive depletion interaction between the external barrier and larger species in the binary mixture causes the mixture to phase separate. At higher volume fractions, a pure phase of larger particles forms near the potential barrier, and the local density of this pure phase is high enough that a face centered cubic crystalline domain is formed at this region. This crystalline phase diffuses perpendicular to the external po…
Using a novel approximation scheme within the convective diffusion (two body Smoluchowski) equation framework, we unveil the shear-driven aggregation mechanism at the origin of structure-formation in sheared colloidal systems. The theory, verified against numerics and experiments, explains the induction time followed by explosive (irreversible) rise of viscosity observed in charge-stabilized colloidal and protein systems under steady shear. The Arrhenius-type equation with shear derived here, extending Kramers theory in the presence of shear, is the first analytical result clearly showing the …
We numerically study a simple model for thermo-reversible colloidal gelation in which particles can form reversible bonds with a predefined maximum number of neighbors. We focus on three and four maximally coordinated particles, since in these two cases the low valency makes it possible to probe, in equilibrium, slow dynamics down to very low temperatures $T$. By studying a large region of $T$ and packing fraction $ϕ$ we are able to estimate both the location of the liquid-gas phase separation spinodal and the locus of dynamic arrest, where the system is trapped in a disordered non-ergodic sta…
School of Chemistry, Tel Aviv University（特拉维夫大学化学学院）；The Institute of Mathematical Sciences（数学科学研究所）；Homi Bhabha National Institute（霍米·巴巴国家研究所）；University of Haifa（海法大学）
Models of 3D confluent tissue as under-constrained glasses
Department of Physics, Emory University（埃默里大学物理系）；Aix Marseille Univ, Université de Toulon, CNRS, CPT (UMR 7332), Turing Centre for Living systems（艾克斯马赛大学、土伦大学、法国国家科学研究中心、CPT（UMR 7332）、图灵生命系统中心）
Colloidal particles are considered ideal building blocks to produce materials with enhanced physical properties. The state-of-the-art techniques for synthesizing these particles provide control over shape, size, and directionality of the interactions. In spite of these advances, there is still a huge gap between the synthesis of individual components and the management of their spontaneous organization towards the desired structures. The main challenge is the control over the dynamics of self-organization. In their kinetic route towards thermodynamically stable structures, colloidal particles …
We show in simulations that a rich variety of novel orderings such as pinwheel and star states can be realized for colloidal molecular crystal mixtures at rational ratios of the number of colloids to the number of minima from an underlying periodic substrate. These states can have multi-step melting transitions and also show coexistence in which one species disorders while the other species remains orientationally disordered. For other mixtures, only partially ordered or frustrated states form.
The phase behavior of a two-dimensional colloidal system subject to a commensurate triangular potential is investigated. We consider the integer number of colloids in each potential minimum as rigid composite objects with effective discrete degrees of freedom. It is shown that there is a rich variety of phases including ``herring bone'' and ``Japanese 6 in 1'' phases. The ensuing phase diagram and phase transitions are analyzed analytically within variational mean-field theory and supplemented by Monte Carlo simulations. Consequences for experiments are discussed.
We demonstrate both experimentally and theoretically that a colloidal sphere trapped in a static optical tweezer does not come to equilibrium, but rather reaches a steady state in which its probability flux traces out a toroidal vortex. This non-equilibrium behavior can be ascribed to a subtle bias of thermal fluctuations by non-conservative optical forces. The circulating sphere therefore acts as a Brownian motor. We briefly discuss ramifications of this effect for studies in which optical tweezers have been treated as potential energy wells.
Density functional theory is used to study colloidal hard-rod fluids near an individual right-angled wedge or edge as well as near a hard wall which is periodically patterned with rectangular barriers. The Zwanzig model, in which the orientations of the rods are restricted to three orthogonal orientations but their positions can vary continuously, is analyzed by numerical minimization of the grand potential. Density and orientational order profiles, excess adsorptions, as well as surface and line tensions are determined. The calculations exhibit an enrichment [depletion] of rods lying parallel…
The mechanism of diffusing diffusivity predicts that, in environments where the diffusivity changes gradually, the displacement distribution becomes non-Gaussian, even though the mean-squared displacement (MSD) grows linearly with time. Here, we report single-particle tracking measurements of the diffusion of colloidal spheres near a planar substrate. Because the local effective diffusivity is known, we have been able to carry out the first direct test of this mechanism for diffusion in inhomogeneous media.
We demonstrate that particles confined to two dimensions (2d) and subjected to a one-dimensional (1d) periodic potential exhibit a rich phase diagram, with both ``locked floating solids'' and smectic phases. The resulting phases and phase transitions are studied as a function of temperature and potential strength. We find reentrant melting as a function of the potential strength. Our results lead to universal predictions consistent with recent experiments on 2d colloids in the presence of a laser-induced 1d periodic potential.
We experimentally investigate the distribution of the non-equilibrium work done by an external force on a mesoscopic system with many coupled degrees of freedom: a colloidal monolayer mechanically driven across a periodic light field. Since this system mimics the spatiotemporal dynamics of a crystalline surface moving on a corrugated substrate, our results show general properties of the non-equilibrium work distribution of atomically flat surfaces undergoing friction. We address the role of several parameters which can influence the shape of the work distribution, e.g. the number of particles …
Two-dimensional colloidal suspensions exposed to periodic external fields exhibit a variety of molecular crystalline phases. There two or more colloids assemble at lattice sites of potential minima to build new structural entities, referred to as molecules. Using the strength of the potential and the filling fraction as control parameter, phase transition to unconventional orientationally ordered states can be induced. We introduce an approach that focuses at the discrete set of orientational states relevant for the phase ordering. The orientationally ordered states are mapped to classical spi…
The work is devoted to particles dynamics simulation in a colloidal drop, when it dries on a substrate and the triple-phase boundary is fixed. Experimental observations [Deegan R. D. et. al., 2000] show a ring deposition on a solid substrate after full droplet desiccation. This phenomenon of macrolevel is known as coffee ring effect. There are other experiments that show a co-effect at the microlevel. We are talking about the formation of a quasicrystalline structure on the outer part of the ring and occurrence amorphous inner zone of ring [Mar\'ın Á. G. et. al., 2011]. The goal of this work i…
Colloids coupled to a bath of swimming cells generically display enhanced diffusion. This transport dynamics stems from a subtle interplay between the active and passive particles that still resists our understanding despite decades of intense research. Here, we tackle the root of the problem by providing a quantitative characterisation of the single scattering events between a colloid and a bacterium. Based on our experiments, we build a minimal model that quantitatively predicts the geometry of the scattering trajectories, and enhanced colloidal diffusion at long times. This quantitative con…
Using Langevin simulations we examine driven colloids interacting with quenched disorder. For weak substrates the colloids form an ordered state and depin elastically. For increasing substrate strength we find a sharp crossover to inhomogeneous depinning and a substantial increase in the depinning force, analogous to the peak effect in superconductors. The velocity versus driving force curve shows criticality at depinning, with a change in scaling exponent occuring at the order to disorder crossover. Upon application of a sudden pulse of driving force, pronounced transients appear in the disor…
We experimentally investigate the structural behavior of an interacting colloidal monolayer being driven across a decagonal quasiperiodic potential landscape created by an optical interference pattern. When the direction of the driving force is varied, we observe the monolayer to be directionally locked on angles corresponding to the symmetry axes of the underlying potential. At such locking steps we observe a dynamically ordered smectic phase in agreement with recent simulations. We demonstrate, that such dynamical ordering is due to the interaction of particle lanes formed by interstitial an…
Using a phase field crystal model we study the structure and dynamics of a drop of colloidal suspension during evaporation of the solvent. We model an experimental system where contact line pinning of the drop on the substrate is non-existent. Under such carefully controlled conditions, evaporation of the drop produces an ordered or disordered arrangement of the colloidal residue depending on the initial average density of solute and the drying rate. We obtain a non-equilibrium phase boundary showing amorphous and crystalline phases of single component and binary mixtures of colloidal particle…
We report the modifications of the microscopic dynamics of a colloidal glass submitted to shear. We use multispeckle diffusing wave spectroscopy to monitor the evolution of the spontaneous slow relaxation processes after the sample have been submitted to various straining. We show that high shear rejuvenates the system and accelerates its dynamics whereas moderate shear overage the system. We analyze this phenomena within the frame of the Bouchaud's trap model.
Quantitative tracking of features from video images is a basic technique employed in many areas of science. Here, we present a method for the tracking of features that partially overlap, in order to be able to track so-called colloidal molecules. Our approach implements two improvements into existing particle tracking algorithms. Firstly, we use the history of previously identified feature locations to successfully find their positions in consecutive frames. Secondly, we present a framework for non-linear least-squares fitting to summed radial model functions and analyze the accuracy (bias) an…
We investigate the behavior of colloidal particles immersed in a binary liquid mixture of water and 2,6-lutidine in the presence of a chemically patterned substrate. Close to the critical point of the mixture, the particles are subjected to critical Casimir interactions with force components normal and parallel to the surface. Because the strength and sign of these interactions can be tuned by variations in the surface properties and the mixtures temperature, critical Casimir forces allow the formation of highly ordered monolayers but also extend the use of colloids as model systems.
In superionic compounds one component pre-melts providing high ionic conductivity to solid state electrolytes. Here, we find sublattice melting in colloidal crystals of oppositely charged particles that are highly asymmetric in size and charge in salt solutions. The small particles in ionic compounds melt when the temperature increases forming a superionic phase. These delocalized small particles in a crystal of large oppositely charged particles, in contrast to superionic phases in atomic systems, form crystals with non-electroneutral stoichiometric ratios. This generates structures with mult…
Two dimensional suspensions of spherical colloids subject to periodic external fields exhibit a rich variety of molecular crystalline phases. We study in simulations the ground state configurations of dimeric and trimeric systems, that are realized on square and triangular lattices, when either two or three macroions are trapped in each external potential minimum. Bipartite orders of the checkerboard or stripe types are reported together with more complex quadripartite orderings, and the shortcomings of envisioning the colloids gathered in a single potential minimum as a composite rigid object…
Using Brownian dynamics simulations we perform a systematic investigation of the shear-induced migration of colloidal particles subject to Poiseuille flow in both cylindrical and planar geometry. We find that adding an attractive component to the interparticle interaction enhances the migration effect, consistent with recent simulation studies of platelet suspensions. Monodisperse, bidisperse and polydisperse systems are studied over a range of shear rates, considering both steady states and the transient dynamics arising from the onset of flow. For bidisperse and polydisperse systems size seg…
Strongly interacting binary mixtures of superparamagnetic colloidal particles confined to a two-dimensional water-air interface are examined by theory, computer simulation and experiment. The mixture exhibits a partial clustering in equilibrium: in the voids of the matrix of unclustered big particles, the small particles form subclusters with a sponge-like topology which is accompanied by a characteristic small-wave vector peak in the small-small structure factor. This partial clustering is a general phenomenon occurring for strongly coupled negatively non-additive mixtures.
We report an experimental study of the elastic properties of a two-dimensional (2D) colloidal crystal subjected to light-induced substrate potentials. In agreement with recent theoretical predictions [H.H. von Gruenberg and J. Baumgartl, Phys. Rev. E 75, 051406 (2007)] the phonon band structure of such systems can be tuned depending on the symmetry and depth of the substrate potential. Calculations with binary crystals suggest that phononic band engineering can be also performed by variations of the pair potential and thus opens novel perspectives for the fabrication of phononic crystals with …
Using Brownian dynamics (BD) simulations and an analytical approach we investigate the shear-induced, nonequilibrium dynamics of dense colloidal suspensions confined to a narrow slit-pore. Focusing on situations where the colloids arrange in well-defined layers with solidlike in-plane structure, the confined films display complex, nonlinear behavior such as collective depinning and local transport via density excitations. These phenomena are reminiscent of colloidal monolayers driven over a periodic substrate potential. In order to deepen this connection, we present an effective model which ma…
We present experimental confirmation of dynamic facilitation in monodisperse and bidisperse colloidal suspensions near the glass transition volume fraction. Correlations in particle dynamics are seen to exist not only in space (clusters and strings) but also as bubbles in space-time. Quantitatively, highly mobile particles are more likely (than immobile particles) to have nearest neighbors that were highly mobile in immediately preceding times. The interpretation is that a particle's mobility enables or facilitates the subsequent motion of its neighbors. Facilitation is most pronounced at the …
We investigate deposit patterns and associated morphology formed after the evaporation of an aqueous droplet containing mono- and bi-dispersed colloidal particles. In particular, the combined effect of substrate heating and particle diameter is investigated. We employ high-speed visualization, optical microscopy and scanning electron microscopy to characterize the evaporating droplets, particle motion, and deposit morphology, respectively. In the context of mono-dispersed colloidal particles, an inner deposit and a typical ring form for smaller and larger particles, respectively, on a nonheate…
Using the recently developed so-called White Bear version of Rosenfeld's Fundamental Measure Theory we calculate the depletion potentials between a hard-sphere colloidal particle in a solvent of small hard spheres and simple models of geometrically structured substrates: a right-angled wedge or edge. In the wedge geometry, there is a strong attraction beyond the corresponding one near a planar wall that significantly influences the structure of colloidal suspensions in wedges. In accordance with an experimental study, for the edge geometry we find a free energy barrier of the order of several …
We study colloidal particle dynamics of a model glass system using confocal and fluorescence microscopy as the sample evolves from a hard-sphere glass to a liquid with attractive interparticle interactions. The transition from hard-sphere glass to attractive liquid is induced by short-range depletion forces. The development of liquid-like structure is indicated by particle dynamics. We identify particles which exhibit substantial motional events and characterize the transition using the properties of these motional events. As samples enter the attractive liquid region, particle speed during th…
The formation and dynamics of a wide variety of binary two-dimensional ordered structures and superlattices are investigated through a phase field crystal model with sublattice ordering. Various types of binary ordered phases, the phase diagrams, and the grain growth dynamics and structural transformation processes, including the emergence of topological defects, are examined. The results are compared to the ordering and assembly of two-component colloidal systems. Two factors governing the binary phase ordering are identified, the coupling and competition between the length scales of two subl…
Although glassy relaxation is typically associated with disorder, here we report on a new type of glassy dynamics relating to dislocations within 2-D crystals of colloidal dimers. Previous studies have demonstrated that dislocation motion in dimer crystals is restricted by certain particle orientations. Here, we drag an optically trapped particle through such dimer crystals, creating dislocations. We find a two-stage relaxation response where initially dislocations glide until encountering particles that cage their motion. Subsequent relaxation occurs logarithmically slowly through a second pr…
Based on Dynamical Density Functional Theory (DDFT) we investigate a binary mixture of interacting Brownian particles driven over a substrate via a one-dimensional ratchet potential. The particles are modeled as soft spheres where one component carries a classical Heisenberg spin. In the absence of a substrate field, the system undergoes a first-order fluid-fluid demixing transition driven by the spin-spin interaction. We demonstrate that the interplay between the intrinsic spinodal decomposition and time-dependent external forces leads to a novel dynamical instability where stripes against th…
We examine colloidal particles driven over a periodic muffin tin substrate using numerical simulations. In the absence of a driving force this system exhibits a rich variety of commensurate and incommensurate static phases in which topological defects can form domain walls, ordered stripes, superlattices, and disordered patchy regimes as a function of the filling fraction. When an external drive is applied, these different static phases generate distinct dynamical responses. At incommensurate fillings the flow generally occurs in the form of localized pulses or solitons correlated with the mot…
When a liquid film of colloidal solution consisting of particles of different sizes is dried on a substrate, the colloids often stratify, where smaller colloids are laid upon larger colloids. This phenomenon is counter intuitive because larger colloids which have smaller diffusion constant are expected to remain near the surface during the drying process, leaving the layer of larger colloids on top of smaller colloids. Here we show that the phenomenon is caused by the interaction between the colloids, and can be explained by the diffusion model which accounts for the interaction between the co…
Using lubrication theory, drying processes of sessile colloidal droplets on a solid substrate are studied. A simple model is proposed to describe temporal dynamics both the shape of the drop and the volume fraction of the colloidal particles inside the drop. The concentration dependence of the viscosity is taken into account. It is shown that the final shapes of the drops depend on both the initial volume fraction of the colloidal particles and the capillary number. The results of our simulations are in a reasonable agreement with the published experimental data. The computations for the drops…
To gain insight into the kinetics of colloidal gel evolution at low particle volume fractions $ϕ$, we utilize differential dynamic microscopy to investigate particle aggregation, geometric percolation, and the subsequent transition to nonergodic dynamics. We report the emergence of unexpectedly rich multiscale dynamics upon the onset of nonergodicity, which separates the wave vectors $q$ into three different regimes. In the high-$q$ domain, the gel exhibits $ϕ$-independent internal vibrations of fractal clusters. The intermediate-$q$ domain is dominated by density fluctuations at the length sc…
As recently reported [Turiv T. et al., Science, 2013, Vol. 342, 1351], fluctuations in the orientation of the liquid crystal (LC) director can transfer momentum from the LC to a colloid, such that the diffusion of the colloid becomes anomalous on a short time scale. Using video microscopy and single particle tracking, we investigate random thermal motion of colloidal particles in a nematic liquid crystal for the time scales shorter than the expected time of director fluctuations. At long times, compared to the characteristic time of the nematic director relaxation we observe typical anisotropi…
We study the dynamics of colloidal suspensions of hard spheres that are subject to Brownian motion in the overdamped limit. We obtain the time evolution of the self and distinct parts of the van Hove function by means of dynamical density functional theory (DDFT). The free energy model for the hard sphere fluid that we use is the very accurate White Bear II version of Rosenfeld's fundamental measure theory. However, in order to remove interactions within the self part of the van Hove function a non-trivial modification has to be applied to the free energy functional. We compare our theoretical…
The emergence of structure through aggregation is a fascinating topic and of both fundamental and practical interest. Here we demonstrate that self-generated solvent flow can be used to generate long-range attractions on the colloidal scale, with sub-pico Newton forces extending into the millimeter-range. We observe a rich dynamic behavior with the formation and fusion of small clusters resembling molecules, the dynamics of which is governed by an effective conservative energy that decays as $1/r$. Breaking the flow symmetry, these clusters can be made active.
We study bidisperse colloidal suspensions confined within glass microcapillary tubes to model the glass transition in confined cylindrical geometries. We use high speed three-dimensional confocal microscopy to observe particle motions for a wide range of volume fractions and tube radii. Holding volume fraction constant, we find that particles move slower in thinner tubes. The tube walls induce a gradient in particle mobility: particles move substantially slower near the walls. This suggests that the confinement-induced glassiness may be due to an interfacial effect.
Effects of substrate temperature, substrate wettability and particles concentration are experimentally investigated for evaporation of a sessile water droplet containing colloidal particles. Time-varying droplet shapes and temperature of the liquid-gas interface are measured using high-speed visualization and infrared thermography, respectively. The motion of the particles inside the evaporating droplet is qualitatively visualized by an optical microscope and profile of final particle deposit is measured by an optical profilometer. On a non-heated hydrophilic substrate, a ring-like deposit for…
