Attractive Particles Research Articles

Quasi-two-dimensional dispersions of Brownian particles with competitive interactions: phase behavior and structural properties.

Competing short-range attractive (SA) and long range repulsive (LR) particle interactions can be used to describe three-dimensional charge-stabilized colloid or protein dispersions at low added salt concentrations, as well as membrane proteins with interaction contributions mediated by lipid molecules. Using Langevin dynamics (LD) simulations, we determine the generalized phase diagram, cluster shapes and size distributions of a generic quasi-two-dimensional (Q2D) dispersion of spherical SALR particles confined to in-plane motion inside a bulk fluid. The SA and LR interaction parts are modelled by a generalized Lennard-Jones potential and a screened Coulomb potential, respectively. The microstructures of the detected equilibrium and non-equilibrium Q2D phases are distinctly different from those observed in three-dimensional (3D) SALR systems, by exhibiting different levels of hexagonal ordering. We discuss a thermodynamic perturbation theory prediction for the metastable binodal line of a reference system of particles with SA interactions only, which in the explored Q2D-SALR phase diagram region separates cluster from non-clustered phases. The transition from the high-temperature (small SA) dispersed fluid (DF) phase to the lower-temperature equilibrium cluster (EC) fluid phase is characterised by a low-wavenumber peak height of the static structure factor (corresponding to a thermal correlation length of about twice the particle diameter) featuring a distinctly smaller value (≈1.4) than in 3D SALR systems. With decreasing temperature (increasing SA), the cluster morphology changes from disk-like shapes in the equilibrium cluster phase, to double-stranded anisotropic hexagonal cluster segments formed in a cluster-percolated (CP) gel-like phase. This transition can be quantified by a hexagonal order parameter distribution function. The mean cluster size and coordination number of particles in the CP phase are insensitive to changes in the attraction strength.

High moments of the SHE in the clustering regimes

We analyze the high moments of the Stochastic Heat Equation (SHE) via a transformation to the attractive Brownian Particles (BPs), which are Brownian motions interacting via pairwise attractive drift. In those scaling regimes where the particles tend to cluster, we prove a Large Deviation Principle (LDP) for the empirical measure of the attractive BPs. Under the delta(-like) initial condition, we characterize the unique minimizer of the rate function and relate the minimizer to the spacetime limit shapes of the Kardar–Parisi–Zhang (KPZ) equation in the upper tails. The results of this paper are used in the companion paper [75] to prove an n-point, upper-tail LDP for the KPZ equation and to characterize the corresponding spacetime limit shape.

Spontaneous separation of attractive chiral mixtures.

The separation of chiral matter has garnered significant attention due to its wide-ranging applications in biological and chemical processes. In prior researches, particle interactions were predominantly repulsive, but the indiscriminate attraction among particles under attractive interactions makes the separation of mixtures more difficult. The question of whether chiral mixed particles, characterized by attractive effects, can undergo spontaneous separation, remains unresolved. We study a binary mixture of chiral (counterclockwise or clockwise) active particles with attractive interactions. It is demonstrated that attractive chiral particles can undergo spontaneous separation without the aid of any specific strategies. The key factor driving the separation is the attractive interactions, enabling the formation of stable clusters of particles with same chirality. There exist optimal parameters (self-propelled velocity, angular velocity, and packing fraction) at which the separation is optimal. Our results may contribute to a deeper understanding of the mechanisms behind chiral matter separation and potentially catalyze further experimental investigations in this field.

An attractive model: simulating fuzzy dark matter with attractive self-interactions

Abstract Fuzzy Dark Matter (FDM) comprised of ultralight ($m \sim 10^{-22}~\rm {eV}$) boson particles has received significant attention as a viable alternative to Cold Dark Matter (CDM), as it approximates CDM on large scales (≳ 1 Mpc) while potentially resolving some of its small-scale problems via kiloparsec-scale quantum interference. However, the most basic FDM model, with one free parameter (the boson mass), is subject to a tension: small boson masses yield the desired cores of dwarf galaxies but underpredict structure in the Lyman-α forest, while large boson masses render FDM effectively identical to CDM. This Catch-22 problem may be alleviated by considering an axion-like particle with attractive particle self-interactions. We simulate an idealized FDM halo with self-interactions parameterized by an energy decay constant $f \sim 10^{15}~\rm {GeV}$ related to the axion symmetry-breaking conjectured to solve the strong-CP problem in particle physics. We observe solitons, a hallmark of FDM, condensing within a broader halo envelope, and find that the density profile and soliton mass depend on self-interaction strength. We propose generalized formulae to extend those from previous works to include self-interactions. We also investigate a critical mass threshold predicted for strong interactions at which the soliton collapses into a compact, unresolved state. We find that the collapse happens quickly and its effects are initially contained to the central region of the halo.

The ion-activated attractive patchy particle model and its application to the liquid-vapor phase transitions.

Patchy particles are an intriguing subject of study and indeed a model system in the field of soft matter physics. In recent years, patchy particle models have been applied to describe a wide variety of systems, including colloidal crystals, macromolecular interactions, liquid crystals, and nanoparticle assemblies. Given the importance of the topic, rationalizing and capturing the basic features of these models is crucial to their correct application in specific systems. In this study, we extend the ion-activated attractive patchy particles model previously employed to elucidate the phase behavior of protein solutions in the presence of trivalent salts. Our extension incorporates the effect of repulsion between unoccupied and occupied binding sites, depicted as patches. Furthermore, we examine the influence of model parameters on the liquid-vapor coexistence region within the phase diagram, employing numerical methods. A deeper understanding of this model will facilitate a better comprehension of the effects observed in experiments.

Guidelines for biomimetic 3D/4D printing in drug delivery

Four-dimensional printing, sometimes known as 4DP, is becoming an increasingly popular area of study. Utilization of “shrewd” materials in 3D printing considers the making of items that answer non-mechanical boosts (like dampness, electric or attractive fields, UV, temperature, pH, or particle arrangement) by progressively changing their shape after some time, as modified. These things could be printed with a shape-moving component that is constrained by a PC. Gadgets made with 4D printing innovation exploit time as the final aspect in their activity. 4D shrewd designs have been concentrated on in the logical writing for a really long time, much before the coming of 3D printing. Medicine delivery at the nano-, miniature, and full-scale scales have all been investigated utilizing ideas from shape development and self-gathering. This study lays forward a far-reaching set of rules for utilizing biomimetic 3D/4D printing techniques in drug delivery frameworks. Biomimetic 3D/4D printing has arisen as a game-changing method in the field of medicine delivery, considering unmatched accuracy and command over drug discharge qualities. In particular, this study looks at the manners by which 3D and 4D printing are being utilized as prescription delivery techniques and with regards to customized medication in the pharmaceutical business.

Which Coverages of Arc-Shaped Proteins Are Required for Membrane Tubulation?

Arc-shaped BIN/Amphiphysin/Rvs (BAR) domain proteins generate curvature by binding to membranes and induce membrane tubulation at sufficiently large protein coverages. For the amphiphysin N-BAR domain, Le Roux et al., Nat. Commun. 2021, 12, 6550, measured a threshold coverage of 0.44 ± 0.097 for nanotubules emerging from the supported lipid bilayer. In this article, we systematically investigate membrane tubulation induced by arc-shaped protein-like particles with coarse-grained modeling and simulations and determine the threshold coverages at different particle-particle interaction strengths and membrane spontaneous curvatures. In our simulations, the binding of arc-shaped particles induces a membrane shape transition from spherical vesicles to tubules at a particle threshold coverage of about 0.5, which is rather robust to variations of the direct attractive particle interactions or spontaneous membrane curvature in the coarse-grained model. Our study suggests that threshold coverages of around or slightly below 0.5 are a general requirement for membrane tubulation by arc-shaped BAR domain proteins.

Universal properties of repulsive self-propelled particles and attractive driven particles

Motility-induced phase separation (MIPS) is a nonequilibrium phase separation that has a different origin from equilibrium phase separation induced by attractive interactions. Similarities and differences in collective behaviors between these two types of phase separation have been intensely discussed. Here, to study another kind of similarity between MIPS and attraction-induced phase separation under a nonequilibrium condition, we perform simulations of active Brownian particles with uniaxially anisotropic self-propulsion (uniaxial ABPs) in two dimensions. We find that (i) long-range density correlation appears in the homogeneous state; (ii) anisotropic particle configuration appears in MIPS, where the anisotropy removes the possibility of microphase separation suggested for isotropic ABPs [X.-Q. Shi , ]; and (iii) critical phenomena for the anisotropic MIPS presumably belong to the universality class for two-dimensional uniaxial ferromagnets with dipolar long-range interactions. Properties (i)–(iii) are common to the well-studied randomly driven lattice gas (RDLG), which is a particle model that undergoes phase separation by attractive interactions under external driving forces, suggesting that the origin of phase separation is not essential for macroscopic behaviors of uniaxial ABPs and RDLG. Based on the observations in uniaxial ABPs, we construct a coarse-grained Langevin model that shows properties (i)–(iii) and corroborates the generality of the findings. Published by the American Physical Society 2024

Modeling Charge Transport in Flowable Suspension Electrolytes

Flowable suspension electrolytes (FSEs) consist of electrically conductive, redox-active, and/or energy-storing particles suspended in aqueous or non-aqueous electrolyte solutions (supporting salt + solvent). These particles, which can range in size from nanometers to micrometers, are subjected to Brownian forces, hydrodynamic forces, hydrophobic interactions, and van der Walls interactions among others. FSEs may enable electrochemical processes where solid reactants can be integrate with flow cells potentially unlocking new approaches to materials processing (e.g., synthesis, extraction/recovery). For example, FSEs has been demonstrated in redox flow batteries, facilitating higher energy densities without sacrificing independent power and energy scaling However, understanding and controlling charge transport through the deformable particle microstructures, especially under shear, is key to enable desirable current distributions and thus effective electrode utilization.In this presentation, we investigate the impact of interparticle interactions, particle volume fractions, and applied shear rate on charge transport through FSEs. At sufficiently large volume fractions above the percolation threshold and stationary conditions, particle interactions in an FSE can drive the formation of networks that span the cell dimensions and provide electronic transport similar to stationary freestanding porous electrodes. However, under flowing conditions, shear forces can break these networks, hampering charge transport. Conversely, increasing attractive particle interactions or particle concentration can strengthen the particle networks and fortifying charge transport, albeit at the expense of fluid viscosity. To better understand these processes, we model the charge transport through these dynamic particle networks, using a combination of local charge transport models and discrete particle simulations, considering the Peclet number (ratio of shearing to Brownian forces) and Mason number (ratio of shearing to attractive forces). Our results contribute to the development of continuum models for charge transport in FSEs, which, in turn, can facilitate efficient and accurate system-level analysis. Acknowledgments This work was funded by the Skoltech – MIT Next Generation Program.

Phase coexistence implications of violating Newton's third law.

Newton's third law, action = reaction, is a foundational statement of classical mechanics. However, in natural and living systems, this law appears to be routinely violated for constituents interacting in a nonequilibrium environment. Here, we use computer simulations to explore the macroscopic phase behavior implications of breaking microscopic interaction reciprocity for a simple model system. We consider a binary mixture of attractive particles and introduce a parameter that is a continuous measure of the degree to which interaction reciprocity is broken. In the reciprocal limit, the species are indistinguishable, and the system phase separates into domains with distinct densities and identical compositions. Increasing nonreciprocity is found to drive the system to explore a rich assortment of phases, including phases with strong composition asymmetries and three-phase coexistence. Many of the states induced by these forces, including traveling crystals and liquids, have no equilibrium analogs. By mapping the complete phase diagram for this model system and characterizing these unique phases, our findings offer a concrete path forward toward understanding how nonreciprocity shapes the structures found in living systems and how this might be leveraged in the design of synthetic materials.

Flocking without Alignment Interactions in Attractive Active Brownian Particles

Within a simple model of attractive active Brownian particles, we predict flocking behavior and challenge the widespread idea that alignment interactions are necessary to observe this collective phenomenon. Here, we show that even nonaligning attractive interactions can lead to a flocking state. Monitoring the velocity polarization as the order parameter, we reveal the onset of a first-order transition from a disordered phase, characterized by several small clusters, to a flocking phase, where a single flocking cluster is emerging. The scenario is confirmed by studying the spatial connected correlation function of particle velocities, which reveals scale-free behavior in flocking states and exponential-like decay for nonflocking configurations. Our predictions can be tested in microscopic and macroscopic experiments showing flocking, such as animals, migrating cells, and active colloids.

Solitonic-like interactions of counter-propagating clusters of active particles.

This report considers a set of interacting self-propelled particles immersed in a viscous and noisy environment. The explored particle interaction does not distinguish between alignments and anti-alignments of the self-propulsion forces. More specifically, we considered a set of self-propelled apolar aligning attractive particles. Consequently, there is no genuine flocking transition because the system has no global velocity polarization. Instead, another self-organized motion emerges, where the system forms two counter-propagating flocks. This tendency leads to the formation of two counter-propagating clusters for short-range interaction. Depending on the parameters, these clusters interact, exhibiting two of the four classical behaviors of counter-propagating dissipative solitons (which does not imply that a single cluster must be recognized as a soliton). They interpenetrate and continue their movement after colliding or forming a bound state where the clusters remain together. This phenomenon is analyzed using two mean-field strategies: an all-to-all interaction that predicts the formation of the two counter-propagating flocks and a noiseless approximation for cluster-to-cluster interaction, which explains the solitonic-like behaviors. Furthermore, the last approach shows that the bound states are metastables. Both approaches agree with direct numerical simulations of the active-particle ensemble.

Erythrocyte Sedimentation Rate: A Physics-Driven Characterization in a Medical Context.

Erythrocyte (or red blood cell) sedimentation rate (ESR) is a physical derived parameter of blood which is often used in routine health checks and medical diagnosis. For instance, in the case of inflammation, a higher ESR is observed due to the associated increase in fibrinogen and other plasma proteins. It was believed that this increase was due to the formation of larger aggregates of red blood cells (RBCs) caused by the increase in fibrinogen. Indeed, fibrinogen is an agent-fostering aggregation of RBCs and in the Stokes regime-assumed to be observed in blood-larger aggregates sediment faster. However, all models of ESR measurements based on this hypothesis require further specific physical assumptions, not required in any other system. Besides, modern studies in the field of colloidal suspensions have established that attractive particles form percolating aggregates (i.e. aggregates as wide as the container). The sedimentation of these colloids then follows a so-called "colloidal gel collapse". Recently, it has been shown that RBCs actually follow the same behavior. This hypothesis also allows to efficiently and analytically model the sedimentation curve of RBCs, from which robust and physically-meaningful descriptors can be extracted. This manuscript describes how to perform such an analysis, and discusses the benefits of this approach.

Aggregation and disaggregation processes in clusters of particles under flow: Simple numerical and theoretical insights

Aggregation and disaggregation of clusters of attractive particles under flow are studied and highlight the growth of the average steady-state cluster size as a power law of the adhesion number, a dimensionless number that quantifies the ratio of attractive forces to shear stress. Such a power-law scaling results from the competition between aggregation and disaggregation processes, as previously reported. Here we rationalize this behavior through a model based on an energy function, for which minimization yields the power-law exponent in terms of the cluster fractal dimension, in good agreement with the present simulations and with previous works.

Shear thinning of non-Brownian suspensions and its variation at different ambient conditions

Immiscible contaminants are commonly involved in naturally occurring suspensions. The resulting variations in their flow behavior have rarely been evaluated. Here, we investigate the variation in the viscosity of an oil-based two-phase suspension over a period of 2 years, which is exposed to the ambient air at the production stage. We find that the absolute humidity of air, which strongly varies with seasons, causes exchanges of water droplets with the suspension, substantially altering its shear-thinning behavior. Only in winter, when the humidity is low, is the latter close to that of the ideal two-phase suspensions. Our measurements suggest that when the surface roughness of the suspended solid particles is sufficiently low, immersed droplets remain in a free state, effectively increasing repulsion between particles, weakening shear thinning. In contrast, when the roughness is sufficiently high, immersed droplets become trapped on the particle surfaces, inducing an attractive particle interaction via water bridging, enhancing shear thinning.

Nanomaterial Endocytosis: Quantification of Adsorption and Ingestion Mechanisms

The widespread use of nanomaterials in vaccines, therapeutics, and industrial applications creates an increasing demand for understanding their ingestion by living cells. Researchers in the field have called for a more robust understanding of physical/chemical particle–cell interactions and a means to determine the particles ingested per cell. Using superparamagnetic nanobeads, we measured the beads per cell and quantified the kinetics of the receptor-independent endocytosis of particles having seven surface chemistries. Poly(ethylene glycol) (PEG)-coated nanoparticles were ingested less effectively by cultured Chinese hamster ovary (CHO-K1) cells and more effectively by aminated nanoparticles than starch-coated particles. The cells ingested 2 to 4 × 105 of the most attractive particles. The interplay between Van der Waals and coulombic potentials was quantified on the basis of Derjaguin–Landau–Verwey–Overbeek (DLVO) theory modified to include hydration repulsion using physical parameters of the seven surface chemistries. Using dose–response curves for inhibitors of clathrin- or caveolae-dependent ingestion, we quantified how particle surface chemistry determines which endocytic pathway is used by the cell. Such characterization can be useful in predicting nanomaterial uptake in medical and toxicological applications and in the selection of particle surface chemistries for receptor-dependent endocytosis.

Impact of granular inclusions on the phase behavior of colloidal gels.

Colloidal gels formed from small attractive particles are commonly used in formulations to keep larger components in suspension. Despite extensive work characterising unfilled gels, little is known about how the larger inclusions alter the phase behavior and microstructure of the colloidal system. Here we use numerical simulations to examine how larger 'granular' particles can alter the gel transition phase boundaries. We find two distinct regimes depending on both the filler size and native gel structure: a 'passive' regime where the filler fits into already-present voids, giving little change in the transition, and an 'active' regime where the filler no longer fits in these voids and instead perturbs the native structure. In this second regime the phase boundary is controlled by an effective colloidal volume fraction given by the available free volume.

High-throughput nanoscale liposome formation via electrohydrodynamic-based micromixer

Liposomes are one of the most attractive particles in different industries, especially pharmaceutical applications. The main reasons for such a desire for liposomes are nontoxicity, small size, the ability to encapsulate and carry biological components, and finally biocompatibility and biodegradability. The present study aims to simulate the active electrohydrodynamic-based micromixer for the high-throughput formation of nanoscale liposomes. The micromixer consists of two inlets for de-ionized water and one inlet for ethanol with lipid particles. Two configurations of asymmetric electrodes, namely, longitudinal and the array of electrodes, were introduced and examined. Electrodes were placed at the bottom of the mixer, and a direct current electrical field was applied to them. Generated chaotic advection inside the microchannel by the electrical field and, consequently, increasing surface-to-volume ratio is the main reason for the increase in the formation of liposomes. These configurations of electrodes cause the liposome formation occurs at very low voltages, which is the most advantage of the proposed micromixer. The Taguchi method as a statistical method of design of experiment (DOE) was utilized to reduce the number of required simulations. The simulations showed that case 6 had the best mixing index of 0.586 among the studied models. Also, according to the DOE results, the best possible design was found and simulated and a mixing index of 0.743, which has a 5.3% error in comparison to the predicted results.

Energy polydisperse 2d Lennard–Jones fluid in the presence of flow field

The behaviour of energy polydisperse 2d Lennard–Jones fluid (in thin-film geometry) is studied subjected to linear flow field using molecular dynamics simulations. By considering neutral and selective substrates, we systematically explore the effect of flow field on particle ordering as well as response of the system. It is shown that particle density profile, spatial organisation as well as local particle identity ordering in the film are affected. Furthermore, we observe flow-induced melting associated with a decrease of effective interaction parameter, $$\langle \epsilon _i^\mathrm{eff} \rangle $$ , which characterises local neighbourhood identity ordering. In terms of macroscopic response, the systems exhibit both shear thinning and shear thickening, and shear thinning exponent decreases with increasing temperature and eventually attains Netwonian fluid-like behaviour at sufficiently high temperature. The onset of shear thinning is governed by the time scale of structural relaxation of the strongly attractive particles. It is found that the qualitative behaviour of the one-component LJ-fluid and energy polydisperse fluid with neutral substrates are similar in many respects, while the one with selective substrate shows differences. In the case of energy polydisperse system, the effect of having different substrate types is significantly manifested in the density profile near the interface, effective interaction parameter and in viscosity.

Rheological Properties, Particle Size Distribution and Physical Stability of Novel Refined Pumpkin Seed Oil Creams with Oleogel and Lucuma Powder.

This research aimed to develop new hazelnut and pumpkin seed oil-based creams and to assess the effect of different fat and sugar phases on the structure and physical properties of those creams at different refining degrees. In this study, three novel spreadable creams were prepared in a stirred ball-mill: CBS with cocoa butter, pumpkin seed oil and saccharose; OS with pumpkin seed oil and carnauba wax-basedoleogel and saccharose; OLS with oleogel, saccharose and Lucuma powder. OS and CBS creams reached a D90 value lower than 30 µm at 150 min of refining, the OLS cream showed the highest D90 value, with a particle size distribution and a rheological behaviour little affected by the refining time. The OS and CBS creams differed in yield stress, indicating that the attractive particle–particle interactions are affected not only by the particle size, but also by fat composition. Moreover, all the creams showed solid-like behaviour and a good tolerance to deformation rate, a high oil-binding capacity and a good physical stability. Thus, it is possible to reformulate spreadable creams with healthier nutritional profiles.