Jamming Limit Research Articles

Particle morphology effects in random sequential adsorption

The properties of the random sequential adsorption of objects of various shapes on a two-dimensional triangular lattice are studied numerically by means of Monte Carlo simulations. The depositing objects are formed by self-avoiding lattice steps, whereby the size of the objects is gradually increased by wrapping the walks in several different ways. The aim of this work is to investigate the impact of the geometrical properties of the shapes on the jamming density θ_{J} and on the temporal evolution of the coverage fraction θ(t). Our results suggest that the order of symmetry axis of a shape exerts a decisive influence on adsorption kinetics near the jamming limit θ_{J}. The decay of probability for the insertion of a new particle onto a lattice is described in a broad range of the coverage θ by the product between the linear and the stretched exponential function for all examined objects. The corresponding fitting parameters are discussed within the context of the shape descriptors, such as rotational symmetry and the shape factor (parameter of nonsphericity) of the objects. Predictions following from our calculations suggest that the proposed fitting function for the insertion probability is consistent with the exponential approach of the coverage fraction θ(t) to the jamming limit θ_{J}.

Discontinuous Shear Thickening in Cornstarch Suspensions

We study the emergence of discontinuous shear-thickening (DST) in cornstarch, the well know system for this phenomenon, by combining macroscopic rheometry with local Magnetic Resonance Imaging (MRI) measurements. We bring evidence that macroscopic DST is characterized in wide gap with a shear localization, part of the material close to the inner cylinder is flowing and the rest is not. The flow seperates into a low-density flowing and a high-density jammed region. Moreover, the local rheology of the flowing region does not directly reflect DST but, strikingly, is most often shear-thinning. Our data are not consistent with recent theoretical suggestions based on the presumed existence of s-shaped flow curves. Instead, they support that DST should be attributed to the existence of a shear jamming limit at volume fractions quite significantly below random close packing.

Periodic protein adsorption at the gold/biotin aqueous solution interface: evidence of kinetics with time delay.

An oscillatory molecular adsorption pattern of the protein neutravidin from aqueous solution onto gold, in presence of a pre-deposited self assembled mono-molecular biotin film, is reported. Real time surface Plasmon resonance sensing was utilized for evaluation of the adsorption kinetics. Two different fractions were identified: in the initial phase, protein molecules attach irreversibly onto the Biotin ligands beneath towards the jamming limit, forming a neutravidin-biotin fraction. Afterwards, the growth rate exhibits distinct, albeit damped adsorption-desorption oscillations over an extended time span, assigned to a quasi reversibly bound fraction. These findings agree with, and firstly confirm a previously published model, proposing macro-molecular adsorption with time delay. The non-linear dynamic model is applicable to and also resembles non-damped oscillatory binding features of the hetero-catalytic oxidation of carbon monoxide molecules on platinum in the gas phase. An associated surface residence time can be linked to the dynamics and time scale required for self-organization.

Electrical conductivity of a monolayer produced by random sequential adsorption of linear k-mers onto a square lattice.

The electrical conductivity of a monolayer produced by the random sequential adsorption (RSA) of linear k-mers (particles occupying k adjacent adsorption sites) onto a square lattice was studied by means of computer simulation. Overlapping with predeposited k-mers and detachment from the surface were forbidden. The RSA process continued until the saturation jamming limit, p_{j}. The isotropic (equiprobable orientations of k-mers along x and y axes) and anisotropic (all k-mers aligned along the y axis) depositions for two different models-of an insulating substrate and conducting k-mers (C model) and of a conducting substrate and insulating k-mers (I model)-were examined. The Frank-Lobb algorithm was applied to calculate the electrical conductivity in both the x and y directions for different lengths (k=1 - 128) and concentrations (p=0 - p_{j}) of the k-mers. The "intrinsic electrical conductivity" and concentration dependence of the relative electrical conductivity Σ(p) (Σ=σ/σ_{m} for the C model and Σ=σ_{m}/σ for the I model, where σ_{m} is the electrical conductivity of substrate) in different directions were analyzed. At large values of k the Σ(p) curves became very similar and they almost coincided at k=128. Moreover, for both models the greater the length of the k-mers the smoother the functions Σ_{xy}(p),Σ_{x}(p) and Σ_{y}(p). For the more practically important C model, the other interesting findings are (i)for large values of k (k=64,128), the values of Σ_{xy} and Σ_{y} increase rapidly with the initial increase of p from 0 to 0.1; (ii) for k≥16, all the Σ_{xy}(p) and Σ_{x}(p) curves intersect with each other at the same isoconductivity points; (iii) for anisotropic deposition, the percolation concentrations are the same in the x and y directions, whereas, at the percolation point the greater the length of the k-mers the larger the anisotropy of the electrical conductivity, i.e., the ratio σ_{y}/σ_{x} (>1).

Protein-Assisted Assembly of Modular 3D Plasmonic Raspberry-like Core/Satellite Nanoclusters: Correlation of Structure and Optical Properties.

We present a bottom-up assembly route for a large-scale organization of plasmonic nanoparticles (NPs) into three-dimensional (3D) modular assemblies with core/satellite structure. The protein-assisted assembly of small spherical gold or silver NPs with a hydrophilic protein shell (as satellites) onto larger metal NPs (as cores) offers high modularity in sizes and composition at high satellite coverage (close to the jamming limit). The resulting dispersions of metal/metal nanoclusters exhibit high colloidal stability and therefore allow for high concentrations and a precise characterization of the nanocluster architecture in dispersion by small-angle X-ray scattering (SAXS). Strong near-field coupling between the building blocks results in distinct regimes of dominant satellite-to-satellite and core-to-satellite coupling. High robustness against satellite disorder was proved by UV/vis diffuse reflectance (integrating sphere) measurements. Generalized multiparticle Mie theory (GMMT) simulations were employed to describe the electromagnetic coupling within the nanoclusters. The close correlation of structure and optical property allows for the rational design of core/satellite nanoclusters with tailored plasmonics and well-defined near-field enhancement, with perspectives for applications such as surface-enhanced spectroscopies.

Discrete element method for generating random fibre distributions in micromechanical models of fibre reinforced composite laminates

A new approach is presented for generating random distribution of fibres in the representative volume element (RVE) of fibre reinforced composite laminates. The approach is based on discrete element method (DEM) and experimental data of fibre diameter distribution. It overcomes the jamming limit appeared in previous methods and is capable of generating high volume fractions of fibres with random distributions and any specified inter-fibre distances. Statistical analysis is then carried out on the fibre distributions generated within the RVEs, which show good agreement with experiments in all statistics analysed. The effective elastic properties of the generated RVEs are finally analysed by finite element method, which results show more reasonable agreement with the experimental results than previous methods.

Extension of the BMCSL equation of state for hard spheres to the metastable disordered region: Application to the SAFT approach.

A simple modification of the Boublík-Mansoori-Carnahan-Starling-Leland equation of state is proposed for an application to the metastable disordered region. The new model has a positive pole at the jamming limit and can accurately describe the molecular simulation data of pure hard in the stable fluid region and along the metastable branch. The new model has also been applied to binary mixtures hard spheres, and an excellent description of the fluid and metastable branches can be obtained by adjusting the jamming packing fraction. The new model for hard sphere mixtures can be used as the repulsive term of equations of state for real fluids. In this case, the modified equations of state give very similar predictions of thermodynamic properties as the original models, and one can remove the multiple liquid density roots observed for some versions of the Statistical Associating Fluid Theory (SAFT) at low temperature without any modification of the dispersion term.

Sub-Poissonian Statistics of Jamming Limits in Ultracold Rydberg Gases.

Several recent experiments have established by measuring the Mandel Q parameter that the number of Rydberg excitations in ultracold gases exhibits sub-Poissonian statistics. This effect is attributed to the Rydberg blockade that occurs due to the strong interatomic interactions between highly excited atoms. Because of this blockade effect, the system can end up in a state in which all particles are either excited or blocked: a jamming limit. We analyze appropriately constructed random-graph models that capture the blockade effect, and derive formulae for the mean and variance of the number of Rydberg excitations in jamming limits. This yields an explicit relationship between the Mandel Q parameter and the blockade effect, and comparison to measurement data shows strong agreement between theory and experiment.

Implicit frictional-contact model for soft particle systems

We introduce a novel numerical approach for the simulation of soft particles interacting via frictional contacts. This approach is based on an implicit formulation of the Material Point Method, allowing for large particle deformations, combined with the Contact Dynamics method for the treatment of unilateral frictional contacts between particles. This approach is both precise due to the treatment of contacts with no regularization and artificial damping parameters, and robust due to implicit time integration of both bulk degrees of freedom and relative contact velocities at the nodes representing the contact points. By construction, our algorithm is capable of handling arbitrary particle shapes and deformations. We illustrate this approach by two simple 2D examples: a Hertz contact and a rolling particle on an inclined plane. We also investigate the compaction of a packing of circular particles up to a solid fraction well above the jamming limit of hard particles. We find that, for the same level of deformation, the solid fraction in a packing of frictional particles is above that of a packing of frictionless particles as a result of larger particle shape change.

Nonlocal effects in sand flows on an inclined plane.

The flow of sand on a rough inclined plane is investigated experimentally. We directly show that a jammed layer of grains spontaneously forms below the avalanche. Its properties and its relation with the rheology of the flowing layer of grains are presented and discussed. In a second part, we study the dynamics of erosion and deposition solitary waves in the domain where they are transversally stable. We characterize their shapes and velocity profiles. We relate their translational velocity to the stopping height and to the mass trapped in the avalanche. Finally, we use the velocity profile to get insight into the rheology very close to the jamming limit.

Apparent wall slip in non-Brownian hard-sphere suspensions.

We analyze apparent wall slip, the reduction of particle concentration near the wall, in hard-sphere suspensions at concentrations well below the jamming limit utilizing a continuum level diffusion model. The approach extends a constitutive equation proposed earlier with two additional potentials describing the effects of gravitation and wall-particle repulsion. We find that although both mechanisms are shear independent by nature, due to the shear-rate-dependent counter-balancing particle migration fluxes, the resulting net effect is non-linearly shear dependent, causing larger slip at small shear rates. In effect, this shows up in the classically measured flow curves as a mild shear thickening regime at the transition from small to intermediate shear rates.

Modeling Deep Bed Filtration Considering Limited Particle Retention

The classic deep bed filtration model (CDBFM) has been widely used for predicting transport and retention of particulate suspensions in porous media. In the CDBFM, the filtration coefficient function is assumed to be dependent of the retained particle concentration, and the boundary conditions are fixed at the porous media inlet cross section. However, if particle retention is limited, no more retention occurs (filtration coefficient equals zero) in regions where maximum retention (jamming limit) is reached. In this article, a model for deep bed filtration considering limited retention is proposed and analytical solutions are obtained. In cases where jamming limit is reached, the well-known CDBFM and the proposed model significantly differ from each other. Contrary to the CDBFM solutions, the obtained solutions show that concentrations along porous media are highly influenced by maximum retention front, which propagates with velocity independent of filtration coefficient.

Adsorption-desorption processes of polydisperse mixtures on a triangular lattice.

Adsorption-desorption processes of polydisperse mixtures on a triangular lattice are studied by numerical simulations. Mixtures are composed of the shapes of different numbers of segments and rotational symmetries. Numerical simulations are performed to determine the influence of the number of mixture components and the length of the shapes making the mixture on the kinetics of the deposition process. We find that, above the jamming limit, the time evolution of the total coverage of a mixture can be described by the Mittag-Leffler function θ(t)=θ∞-ΔθE[-(t/τ)β] for all the mixtures we have examined. Our results show that the equilibrium coverage decreases with the number of components making the mixture and also with the desorption probability, via corresponding stretched exponential laws. For the mixtures of equal-sized objects, we propose a simple formula for predicting the value of the steady-state coverage fraction of a mixture from the values of the steady-state coverage fractions of pure component shapes.

Macroscopic discontinuous shear thickening versus local shear jamming in cornstarch.

We study the emergence of discontinuous shear thickening (DST) in cornstarch by combining macroscopic rheometry with local magnetic resonance imaging measurements. We bring evidence that macroscopic DST is observed only when the flow separates into a low-density flowing and a high-density jammed region. In the shear-thickened steady state, the local rheology in the flowing region is not DST but, strikingly, is often shear thinning. Our data thus show that the stress jump measured during DST, in cornstarch, does not capture a secondary, high-viscosity branch of the local steady rheology but results from the existence of a shear jamming limit at volume fractions quite significantly below random close packing.

Pressure-driven suspension flow near jamming.

We report here magnetic resonance imaging measurements performed on suspensions with a bulk solid volume fraction (ϕ_{0}) up to 0.55 flowing in a pipe. We visualize and quantify spatial distributions of ϕ and velocity across the pipe at different axial positions. For dense suspensions (ϕ_{0}>0.5), we found a different behavior compared to the known cases of lower ϕ_{0}. Our experimental results demonstrate compaction within the jammed region (characterized by a zero macroscopic shear rate) from the jamming limit ϕ_{m}≈0.58 at its outer boundary to the random close packing limit ϕ_{rcp}≈0.64 at the center. Additionally, we show that ϕ and velocity profiles can be fairly well captured by a frictional rheology accounting for both further compaction of jammed regions as well as normal stress differences.

Emerging quasi-0D states at vanishing total entropy of the 1D hard sphere system: A coarse-grained similarity to the car parking problem

A coarse-grained system of one-dimensional (1D) hard spheres (HSs) is created using the Delaunay tessellation, which enables one to define the quasi-0D state. It is found from comparing the quasi-0D and 1D free energy densities that a frozen state due to the emergence of quasi-0D HSs is thermodynamically more favorable than fluidity with a large-scale heterogeneity above crossover volume fraction of $\phi_c=e/(1+e)=0.731\cdots$, at which the total entropy of the 1D state vanishes. The Delaunay-based lattice mapping further provides a similarity between the dense HS system above $\phi_c$ and the jamming limit in the car parking problem.

Kinetics of deposition of oriented superdisks

We use numerical Monte Carlo simulation to study the kinetics of the deposition of oriented superdisks, bounded by the Lame curves of the form |x|(2p)+|y|(2p)=1 on a regular planar substrate. Recently, it was shown that the maximum packing density as well as jamming density ρ(J) exhibit a discontinuous derivative at p=0.5 when the shape changes from convex to concave form. By careful examination of the late-stage approach to the jamming limit, we find that the leading term in the temporal development is also nonanalytic at p=0.5 and offer heuristic excluded-area arguments for this behavior.

Optimization of the monolayer growth in adsorption-desorption processes

Kinetics of the deposition process of dimers in the presence of desorption is studied by Monte Carlo method on a one-dimensional lattice. The aim of this work is to investigate how do various temporal dependencies of the desorption rate hasten or slow down the deposition process. The growth of the coverage θ(t) above the jamming limit to its steady-state value θ(∞) is analyzed when the desorption probability P(des) decreases both stepwise and linearly (continuously) over a certain time domain. We report a numerical evidence that the time needed for a system to reach the given coverage θ can be significantly reduced if P(des) decreases in time. Finally, a self-consistent optimization procedure, when the probability P(des) depends on the current coverage density θ(t), is formulated and tested. The present model reproduces qualitatively the densification kinetics and the memory effects of vibrated granular materials. Our results suggest that the process of vibratory compaction of granular materials can be optimized by using a time dependent intensity of external excitations.

Equilibrium theory of the hard sphere fluid and glasses in the metastable regime up to jamming. II. Structure and application to hopping dynamics

Building on the equation-of-state theory of Paper I, we construct a new thermodynamically consistent integral equation theory for the equilibrium pair structure of 3-dimensional monodisperse hard spheres applicable up to the jamming transition. The approach is built on a two Yukawa generalized mean spherical approximation closure for the direct correlation function (DCF) beyond contact that reproduces the exact contact value of the pair correlation function and isothermal compressibility. The detailed construction of the DCF is guided by the desire to capture its distinctive features as jamming is approached. Comparison of the theory with jamming limit simulations reveals good agreement for many, but not all, of the key features of the pair correlation function. The theory is more accurate in Fourier space where predictions for the structure factor and DCF are accurate over a wide range of wavevectors from significantly below the first cage peak to very high wavevectors. New features of the equilibrium pair structure are predicted for packing fractions below jamming but well above crystallization. For example, the oscillatory DCF decays very slowly at large wavevectors for high packing fractions as a consequence of the unusual structure of the radial distribution function at small separations. The structural theory is used as input to the nonlinear Langevin equation theory of activated dynamics, and calculations of the alpha relaxation time based on single particle hopping are compared to recent colloid experiments and simulations at very high volume fractions.

Random Parking, Euclidean Functionals, and Rubber Elasticity

We study subadditive functions of the random parking model previously analyzed by the second author. In particular, we consider local functions $S$ of subsets of $\mathbb{R}^d$ and of point sets that are (almost) subadditive in their first variable. Denoting by $\xi$ the random parking measure in $\mathbb{R}^d$, and by $\xi^R$ the random parking measure in the cube $Q_R=(-R,R)^d$, we show, under some natural assumptions on $S$, that there exists a constant $\bar{S}\in \mathbb{R}$ such that % $$ \lim_{R\to +\infty} \frac{S(Q_R,\xi)}{|Q_R|}\,=\,\lim_{R\to +\infty}\frac{S(Q_R,\xi^R)}{|Q_R|}\,=\,\bar{S} $$ % almost surely. If $\zeta \mapsto S(Q_R,\zeta)$ is the counting measure of $\zeta$ in $Q_R$, then we retrieve the result by the second author on the existence of the jamming limit. The present work generalizes this result to a wide class of (almost) subadditive functions. In particular, classical Euclidean optimization problems as well as the discrete model for rubber previously studied by Alicandro, Cicalese, and the first author enter this class of functions. In the case of rubber elasticity, this yields an approximation result for the continuous energy density associated with the discrete model at the thermodynamic limit, as well as a generalization to stochastic networks generated on bounded sets.