A simulation model is presented, comprising elastic spheres with a short range attraction. Besides conservative forces, radial- and shear friction, and radial noise are added. The model can be used to simulate colloids, granular solids and powders, and the parameters may be related to experimental systems via the range of attraction and the adhesion energy. The model shares the simplicity and speed of Dissipative Particle Dynamics (DPD), yet the predictions are rather non-trivial. We demonstrate that the model predicts the correct scaling relations for fracture of granular solids, and we present a schematic phase diagram. This shows liquid-vapor coexistence for sufficiently large interaction range, with a surface tension that follows Ising criticality. For smaller interaction range only solid-vapor coexistence is found, but for very small attractive interaction range stable liquid-vapor coexistence reappears due to pathological stability of the solid phase. At very low temperature the model forms a glassy state.
A new potential of mean force is proposed for colloidal dispersions, which is obtained from coarse grained, pair interactions between colloidal particles formed by the explicit grouping of particles that are themselves groups of atoms and molecules. Using numerical simulations, we start by constructing colloidal particles made up of 250 mesoscopic particles joined by springs and interacting with each other through short range forces. Afterward we proceed to model several colloidal concentrations and obtain the colloidal particles pair correlation function, from which we derive the potential of…
A model is presented for the solution of electrokinetic phenomena of colloidal suspensions in fluid mixtures. We solve the discrete Boltzmann equation with a BGK collision operator using the lattice Boltzmann method to simulate binary fluid flows. Solvent-solvent and solvent-solute interactions are implemented using a pseudopotential model. The Nernst-Planck equation, describing the kinetics of dissolved ion species, is solved using a finite difference discretization based on the link-flux method. The colloids are resolved on the lattice and coupled to the hydrodynamics and electrokinetics thr…
We propose a method to analyze the dynamics of systems exhibiting slow relaxation which is based on mesoscopic non-equilibrium thermodynamics. The method allows us to obtain kinetic equations of the Fokker-Planck type for the probability functional and their corresponding Langevin equations. Our results are compared with the ones obtained by other authors.
The constituents of soft matter systems such as colloidal suspensions, emulsions, polymers, and biological tissues undergo microscopic random motion, due to thermal energy. They may also experience drift motion correlated over mesoscopic or macroscopic length scales, \textit{e.g.} in response to an internal or applied stress or during flow. We present a new method for measuring simultaneously both the microscopic motion and the mesoscopic or macroscopic drift. The method is based on the analysis of spatio-temporal cross-correlation functions of speckle patterns taken in an imaging configuratio…
We combine experiments and theory to investigate the dynamics and orientational fluctuations of ferromagnetic microellipsoids that form a ribbon-like structure due to attractive dipolar forces. When assembled in the ribbon, the ellipsoids displays orientational thermal uctuations with an amplitude that can be controlled via application of an in-plane magnetic field. We use video microscopy to investigate the orientational dynamics in real time/space. Theoretical arguments are used to derive an analytical expression that describes how the distribution of the different angular configurations dep…
Nonreciprocal effective interaction forces can occur between mesoscopic particles in colloidal suspensions that are driven out of equilibrium. These forces violate Newton's third law actio=reactio on coarse-grained length and time scales. Here we explore the statistical mechanics of Brownian particles with nonreciprocal effective interactions. Our model system is a binary fluid mixture of spherically symmetric, diffusiophoretic mesoscopic particles, and we focus on the time-averaged particle pair- and triplet-correlation functions. Based on the many-body Smoluchowski equation we develop a micr…
The study of competitive and cooperative adsorption of functionalized molecules such as polymers, rheology modifiers and surfactant molecules on colloidal particles immersed in a solvent is undertaken using coarse grained, dissipative particle dynamics simulations. The results show that a complex picture emerges from the simulations, one where dispersants and surfactants adsorb cooperatively up to certain concentrations, on colloidal particles, but as the surfactant concentration increases it leads to dispersant desorption. The presence of rheology modifying agents in the colloidal dispersion …
Chemotaxis is the response of a particle to a gradient in the chemical composition of the environment. While it was originally observed for biological organisms, it is of great interest in the context of synthetic active particles such as nanomotors. Experimental demonstration of chemotaxis for chemically-powered colloidal nanomotor was reported in the literature in the context of chemo-attraction in a still fluid or in a microfluidic channel where the gradient is sustained by a specific inlet geometry. In this work, we use mesoscopic particle-based simulations of the colloid and solvent to de…
Simulations of colloidal suspensions consisting of mesoscopic particles and smaller species such as ions or depletants are computationally challenging as different length and time scales are involved. Here, we introduce a machine learning (ML) approach in which the degrees of freedom of the microscopic species are integrated out and the mesoscopic particles interact with effective many-body potentials, which we fit as a function of all colloid coordinates with a set of symmetry functions. We apply this approach to a colloid-polymer mixture. Remarkably, the ML potentials can be assumed to be ef…
A novel method to investigate the compaction behaviour of cohesive powders is presented. As a sample, a highly porous agglomerate formed by random ballistic deposition (RBD) of micron sized spherical particles is used. A nanomanipulator deforms this small structure under scanning electron microscope observation, allowing for the tracking of individual particle motion. Defined forces are applied and the resulting deformations are measured. The hereby obtained results are compared to results from threedimensional discrete element simulations as well as macroscopic compaction experiments. Relevan…
We demonstrate that the active thermocapillary stresses induced by multiple microbubbles offer simple routes to directed self-assembly and complex but controllable micromanipulation of mesoscopic colloidal particles embedded in a liquid. The microbubbles are nucleated on a liquid-glass interface using optical tweezers. The flow around a single bubble causes self-assembly of the particles in rings at the bubble-base, while an asymmetric temperature profile generated across the bubble interface breaks the azimuthal symmetry of the flow, and induces simultaneous accumulation and repulsion of part…
We compute the electrostatic potential at the surface, or zeta potential $ζ$, of a charged particle embedded in a colloidal suspension using a hybrid mesoscopic model. We show that for weakly perturbing electric fields, the value of $ζ$ obtained at steady state during electrophoresis is statistically indistinguishable from $ζ$ in thermodynamic equilibrium. We quantify the effect of counterions concentration on $ζ$. We also evaluate the relevance of the lattice resolution for the calculation of $ζ$ and discuss how to identify the effective electrostatic radius.
We present the self-dynamics of protein amino acids of hydrated lysozyme powder around the physiological temperature by means of molecular dynamics (MD) simulations. The self-intermediate scattering functions (SISF) of the amino acid residue center-of-mass and of the protein hydrogen atoms display a logarithmic decay over 3 decades of time, from 2 picoseconds to 2 nanoseconds, followed by an exponential alpha-relaxation. This kind of slow dynamics resembles the relaxation scenario within the beta-relaxation time range predicted by the mode coupling theory (MCT) in the vicinity of higher-order …
The ability to assemble mesoscopic colloidal lattices above a surface is important for fundamental studies related with nucleation and crystallization, but also for a variety of technological applications in photonics and micro-engineering. Current techniques based on particle sedimentation above a lithographic template are limited by a slow deposition process and by the use of static templates, which make difficult to implement fast annealing procedures. Here it is demonstrated a method to realize and anneal a series of colloidal lattices displaying triangular, honeycomb or kagome-like symmet…
A continuum theory is employed to numerically study the equilibrium orientation and defect structures of a circular cylindrical particle with flat ends under a homeotropic anchoring condition in a uniform nematic medium. Different aspect ratios of this colloidal geometry from thin discotic to long rod-like shapes and several colloidal length scales ranging from mesoscale to nanoscale are investigated. We show that the equilibrium state of this colloidal geometry is sensitive to the two geometrical parameters: aspect ratio and length scale of the particle. For a large enough mesoscopic particle…
We study the response of a nematic colloidal dispersion of rods to a driven probe particle which is dragged with high speed through the dispersion perpendicular to the nematic director. In front of the dragged particle, clusters of rods are generated which rhythmically grow and dissolve by rotational motion. We find evidence for a mesoscopic cluster-cluster correlation length, {\em independent} of the imposed drag speed. Our results are based on non-equilibrium Brownian dynamics computer simulations and in line with a dynamical scaling theory.
When strained beyond the linear regime, soft colloidal glasses yield to steady-state plastic flow in a way that is similar to the deformation of conventional amorphous solids. Due to the much larger size of the colloidal particles with respect to the atoms comprising an amorphous solid, colloidal glasses allow to obtain microscopic insight into the nature of the yielding transition, as we illustrate here combining experiments, atomistic simulations, and mesoscopic modeling. Our results unanimously show growing clusters of non-affine deformation percolating at yielding. In agreement with percol…
Tap density of a granular powder is often linked to the flowability via Carr Index that measures how tight a powder can be packed, under an assumption that more easily packed powders usually flow poorly. Understanding how particles are packed is important for revealing why a powder flows better than others. There are two types of empirical equations that were proposed to fit the experimental data of packing fractions vs. numbers of taps in literature: The inverse logarithmic and the stretched exponential. Using the rate process theory and the free volume concept, we obtain the tap density equa…
We study the melting behavior of charged colloidal crystals, using a simulation technique that combines a continuous mean-field Poisson-Boltzmann description for the microscopic electrolyte ions with a Brownian-dynamics simulation for the mesoscopic colloids. This technique ensures that many-body interactions between the colloids are fully taken into account, and thus allows us to investigate how many-body interactions affect the solid-liquid phase behavior of charged colloids. Using the Lindemann criterion, we determine the melting line in a phase-diagram spanned by the colloidal charge and t…
The viscosity concept of thermal systems is borrowed to describe the flowability of granular powders in this article with the granular temperature is defined analogously. Eyrings rate process theory and free volume concept, which have been proved to be very powerful in dealing with many thermally activated phenomena in a wide variety of fields, are utilized to derive viscosity equations of granular powders under a simple shear. The obtained viscosity equations are examined only with empirical experimental observations in describing powder flowability, due to the lack of instruments and methodo…
Attractive colloidal gels display a solid-to-fluid transition as shear stresses above the yield stress are applied. This shear-induced transition is involved in virtually any application of colloidal gels. It is also crucial for controlling material properties. Still, in spite of its ubiquity, the yielding transition is far from understood, mainly because rheological measurements are spatially averaged over the whole sample. Here, the instrumentation of creep and oscillatory shear experiments with high-frequency ultrasound opens new routes to observing the local dynamics of opaque attractive c…
Systems in which a short-ranged attraction and long-ranged repulsion compete are intrinsically frustrated, leading their structure and dynamics to be dominated either by mesoscopic order or by metastable disorder. Here we report the latter case in a colloidal system with long-ranged electrostatic repulsions and short-ranged depletion attractions. We find a variety of states exhibiting slow non-diffusive dynamics: a gel, a glassy state of clusters, and a state reminiscent of a Wigner glass. Varying the interactions, we find a continuous crossover between the Wigner and cluster glassy states, an…
We study many-particle diffusion in 2D colloidal suspensions with full hydrodynamic interactions through a novel mesoscopic simulation technique. We focus on the behaviour of the effective scaled tracer and collective diffusion coefficients $D_T(ρ) / D_0$ and $D_C(ρ) / D_0$, where $D_0$ is the single-particle diffusion coefficient, as a function of the density of the colloids $ρ$. At low Schmidt numbers $Sc={\cal O}(1)$, we find that hydrodynamics has essentially no effect on the behaviour of $D_T(ρ)/D_0$. At larger $Sc$, $D_T(ρ)/D_0$ is enhanced at all densities, although the differences comp…
We develop a mesoscopic field theory for the collective nonequilibrium dynamics of multicomponent mixtures of interacting active (i.e., motile) and passive (i.e., nonmotile) colloidal particles with isometric shape in two spatial dimensions. By a stability analysis of the field theory, we obtain equations for the spinodal that describes the onset of a motility-induced instability leading to cluster formation in such mixtures. The prediction for the spinodal is found to be in good agreement with particle-resolved computer simulations. Furthermore, we show that in active-passive mixtures the spi…
An analytical description of polymer melts and their mixtures as liquids of interacting soft colloidal particles is obtained from liquid-state theory. The derived center-of-mass pair correlation functions with no adjustable parameters reproduce those computed from united atom molecular dynamics simulations. The coarse-grained description correctly bridges micro- and mesoscopic fluid properties. Molecular dynamics simulations of soft colloidal particles interacting through the calculated effective pair potentials are consistent with data from microscale simulations and analytical formulas.
This preliminary study presents a simple modulation scheme to dynamically create time-averaged optical potentials to trap colloidal particles using acousto-optical modulation. The method provides access to control experimentally relevant parameters of a tunable double-well potential. We show experimental data successfully adjusting the trapping distance in the range 20-2000 nm and discuss situations arising when reconstructing time-averaged optical potentials from trapped particle data. This is the first step towards studying colloidal particles in dynamically modulated optical potentials to e…
We use a mesoscopic simulation technique to study the effect of short-ranged inter-particle attraction on the steady-state sedimentation of colloidal suspensions. Attractions increase the average sedimentation velocity $v_s$ compared to the pure hard-sphere case, and for strong enough attractions, a non-monotonic dependence on the packing fraction $ϕ$ with a maximum velocity at intermediate $ϕ$ is observed. Attractions also strongly enhance hydrodynamic velocity fluctuations, which show a pronounced maximum size as a function of $ϕ$. These results are linked to a complex interplay between hydr…
Colloidal crystals are of extreme importance for applied research, such as photonic crystals technology, and for fundamental studies in statistical mechanics. Long range attractive interactions, such as capillary forces, can drive the spontaneous assembly of such mesoscopic ordered structures. However long range attractive forces are very rare in the colloidal realm. Here we report a novel strong and long ranged attraction induced by a thermal gradient in the presence of a wall. Switching on and off the thermal gradient we can rapidly and reversibly form stable hexagonal 2D crystals. We show t…
Very recently, the construction of twist actuators from magnetorheological gels and elastomers has been suggested. These materials consist of magnetizable colloidal particles embedded in a soft elastic polymeric environment. The twist actuation is enabled by a net chirality of the internal particle arrangement. Upon magnetization by a homogeneous external magnetic field, the systems feature an overall torsional deformation around the magnetization direction. Starting from a discrete minimal mesoscopic model set-up we work towards a macroscopic characterization. The two scales are linked by ide…
Chemically powered self-propelled colloids generate a motor force by converting locally a source of energy into directed motion, a process that has been explored both in experiments and in computational models. The use of active colloids as building blocks for nanotechnology opens the doors to interesting applications, provided we understand the behaviour of these elementary constituents. We build a consistent mesoscopic simulation model for self-propelled colloids of complex shape with the aim of resolving the coupling between their translational and rotational motion. Considering a passive L…
Colloidal systems find important applications ranging from fabrication of photonic crystals to direct probing of phenomena typically encountered in atomic crystals and glasses. New applications - such as nanoantennas, plasmonic sensors, and nanocircuits - pose a challenge of achieving sparse colloidal assemblies with tunable interparticle separations that can be controlled at will. We demonstrate reconfigurable multiscale interactions and assembly of colloids mediated by defects in cholesteric liquid crystals that are probed by means of laser manipulation and three-dimensional imaging. We find…
We study mutual alignment and interactions between colloidal particles of dissimilar shapes and dimensions when dispersed in a nematic host fluid. Convex pentagonal and concave starfruit-shaped nanoprisms and microspheres induce dipolar or quadrupolar director structures. The ensuing elastic pair interactions between microspheres and nanoprisms are highly dependent on the nanoparticle shape being omnidirectionally attractive for convex prisms but strongly anisotropic for concave prisms. Elastic deformations due to spherical particles cause well-defined alignment of complex-shaped nanoparticles…
Colloidal particles dispersed in a liquid crystal lead to distortions of the director field. The distortions are responsible for long-range effective colloidal interactions whose asymptotic behaviour is well understood. The short distance behaviour of the interaction, however, is sensitive to the structure and dynamics of the topological defects nucleated near the colloidal particles in the strong anchoring regime. The full non-linear theory is required in order to determine the interaction at short separations. Spherical colloidal particles with sufficiently strong planar degenerate anchoring…
We investigate excluded-volume effects in a bidisperse colloidal suspension near a flexible interface. Inspired by a recent experiment by Dinsmore et al. (Phys. Rev, Lett. 80, 409 (1998)), we study the adsorption of a mesoscopic bead on the surface and show that depletion forces could in principle lead to particle encapsulation. We then consider the effect of surface fluctuations on the depletion potential itself and construct the density profile of a polymer solution near a soft interface. Surprisingly we find that the chains accumulate at the wall, whereas the density displays a deficit of p…
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 …
Colloidal particles disturb the alignment of rod-like molecules of liquid crystals, giving rise to long-range interactions that minimize the free energy of distorted regions. Particle shape and topology are known to guide this self-assembly process. However, how chirality of colloidal inclusions affects these long-range interactions is unclear. Here we study the effects of distortions caused by chiral springs and helices on the colloidal self-organization in a nematic liquid crystal using laser tweezers, particle tracking and optical imaging. We show that chirality of colloidal particles inter…
A mesoscopic theory for the primitive model of ionic systems is developed for arbitrary size, $λ=σ_+/σ_-$, and charge, $Z=e_+/|e_-|$, asymmetry. Our theory is an extension of the theory we developed earlier for the restricted primitive model. The case of extreme asymmetries $λ\to\infty$ and $Z \to\infty$ is studied in some detail in a mean-field approximation. The phase diagram and correlation functions are obtained in the asymptotic regime $λ\to\infty$ and $Z \to\infty$, and for infinite dilution of the larger ions (volume fraction $n_p\sim 1/Z$ or less). We find a coexistence between a very …
We investigate the universal orientation-dependent interactions between non-spherical colloidal particles immersed in a critical solvent by studying the instructive paradigm of a needle embedded in bounded two-dimensional Ising models at bulk criticality. For a needle in an Ising strip the interaction on mesoscopic scales depends on the width of the strip and the length, position, and orientation of the needle. By lattice Monte Carlo simulations we evaluate the free energy difference between needle configurations being parallel and perpendicular to the strip. We concentrate on small but noneth…
A mesoscopic hydrodynamic model to simulate synthetic self-propelled Janus particles which is thermophoretically or diffusiophoretically driven is here developed. We first propose a model for a passive colloidal sphere which reproduces the correct rotational dynamics together with strong phoretic effect. This colloid solution model employs a multiparticle collision dynamics description of the solvent, and combines potential interactions with the solvent, with stick boundary conditions. Asymmetric and specific colloidal surface is introduced to produce the properties of self-phoretic Janus part…
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 …
The macroscopic mechanical properties of densely packed coagulated colloidal particle gels strongly depend on the local arrangement of the powder particles on length scales of a few particle diameters. Heterogeneous microstructures exhibit up to one order of magnitude higher elastic properties and yield strengths than their homogeneous counterparts. The microstructures of these gels are analyzed by the straight path method quantifying quasi-linear particle arrangements of particles. They show similar characteristics than force chains bearing the mechanical load in granular material. Applying t…
To elucidate mechanisms of mesoscopic turbulence exhibited by active particles, we experimentally study turbulent states of non-living self-propelled particles. We realize an experimental system with dense suspensions of asymmetrical colloidal particles (Janus particles) self-propelling on a two-dimensional surface under an AC electric field. Velocity fields of the Janus particles in the crowded situation can be regarded as a sort of turbulence because it contains many vortices and their velocities change abruptly. Correlation functions of their velocity field reveal the coexistence of polar a…
Microscopy and particle-based simulations are both powerful techniques to study aggregated particulate matter such as colloidal gels. The data provided by these techniques often contains information on a wide array of length scales, but structural analysis methods typically focus on the local particle arrangement, even though the data also contains information about the particle network on the mesoscopic length scale. In this paper, we present a MATLAB software package for quantifying mesoscopic network structures in colloidal samples. ArGSLab (Arrested and Gelated Structures Laboratory) extra…
We investigate the dependence of the stickiness parameters $t_{ij}=1/(12τ_{ij})$ -- where the $τ_{ij}$ are the conventional Baxter parameters -- on the solute diameters $σ_{i}$ and $σ_{j}$ in multicomponent sticky hard sphere (SHS) models for fluid mixtures of mesoscopic neutral particles. A variety of simple but realistic interaction potentials, utilized in the literature to model \textit{short-ranged attractions} present in real solutions of colloids or reverse micelles, is reviewed. We consider: i) van der Waals attractions, ii) hard-sphere-depletion forces, iii) polymer-coated colloids, iv…
The possibility of prescribing local interactions between nano- and microscopic components that direct them to assemble in a predictable fashion is a central goal of nanotechnology research. In this article we advance a new paradigm in which self-assembly of DNA-functionalized colloidal particles is programmed using linker oligonucleotides dispersed in solution. We find a phase diagram that is surprisingly rich compared to phase diagrams typical of other DNA-functionalized colloidal particles that interact by direct hybridization, including a re-entrant melting transition upon increasing linke…
We consider depletion effects of a pear-shaped colloidal particle in a hard-sphere solvent, for two different model realisations of the pear-shaped colloidal particle. The two models are the pear hard Gaussian overlap (PHGO) particles and the hard pears of revolution (HPR). The motivation for this study is to provide a microscopic understanding for the substantially different mesoscopic self-assembly properties of these pear-shaped colloids, in dense suspensions, that have been reported in the first part of this series. This is done by determining the differing depletion attraction via MC simu…
One of the major shortcomings of discrete element modelling (DEM) is the computational cost required when the number of particles is huge, especially for fine powders and/or industry scale simulations. This study investigates the scaling of model parameters that is necessary to produce scale independent predictions for cohesionless and cohesive solid under quasi-static simulation of confined compression and unconfined compression to failure in uniaxial test. A bilinear elasto-plastic adhesive frictional contact model was used. The results show that contact stiffness (both normal and tangential…
We present a mesoscopic hydrodynamic description of the dynamics of colloidal suspensions. We consider the system as a gas of Brownian particles suspended in a Newtonian heat bath subjected to stationary non-equilibrium conditions imposed by a velocity field. Using results already obtained in previous studies in the field by means of a generalized Fokker-Planck equation, we obtain a set of coupled differential equations for the local diffusion current and the evolution of the total stress tensor. We find that the dynamic shear viscosity of the system contains contributions arising from the fin…
