Suspensions Of Active Particles Research Articles

A three-dimensional flow-electrochemistry coupling model for optimizing the channel configuration of lithium slurry redox flow battery

Lithium slurry redox flow batteries (SRFBs) are a promising candidate for scalable energy storage systems. The section is one of the most basic elements of the flow field. The battery performance optimization based on the section reconstruction is helpful to improve the flow distribution of active particle suspensions in flow channel, reduce the edge slurry retention, and enhance the reaction uniformity. Here, a three-dimensional numerical model of SRFB is established, and its accuracy is verified by experiments. Through multiphysics field simulation, it is proved that the rectangular section is more suitable for SRFB than the triangular and circular sections for the flow channels, but the velocity distribution is elliptical and decreases along the surrounding edge area. Such a rectangular section reconfiguration, which conforms to the velocity distribution characteristics of the slurry, is beneficial to improve the speed of the slurry edge and promote the overall uniform distribution of the slurry. Specifically, the top-arc bottom rectangular design (A1) demonstrates the best comprehensive performance. The influence of flow rates on the slurry distribution is examined. The results show that the slurry has a relatively low pressure drop and a more uniform distribution when the inlet flow rate is approximately 30 ml min−1.

Universal Poisson statistics of a passive tracer diffusing in dilute active suspensions.

The statistics of a passive tracer immersed in a suspension of active particles (swimmers) is derived from first principles by considering a perturbative expansion of the tracer interaction with the microscopic swimmer field. To first order in the swimmer density, the tracer statistics is shown to be exactly represented by a spatial Poisson process combined with independent tracer-swimmer scattering events, rigorously reducing the multiparticle dynamics to two-body interactions. The Poisson representation is valid in any dimension, for arbitrary interaction forces and for a large class of swimmer dynamics. The framework not only allows for the systematic calculation of the tracer statistics in various dynamical regimes but highlights in particular surprising universal features that are independent of the swimmer dynamics such as a time-independent velocity distribution.

Phase separation of passive particles in active liquids.

The transport properties of colloidal particles in active liquids have been studied extensively. It has led to a deeper understanding of the interactions between passive and active particles. However, the phase behavior of colloidal particles in active media has received little attention. Here, we present a combined experimental and numerical investigation of passive colloids dispersed in suspensions of active particles. Our study reveals dynamic clustering of colloids in active media due to an interplay of activity and attractive effective potential between the colloids. The strength of the effective potential is set by the size ratio of passive particles to the active ones. As the relative size of the passive particles increases, the effective potential becomes stronger and the average size of the clusters grows. The simulations reveal a macroscopic phase separation at sufficiently large size ratios. We will discuss the effect of density fluctuations of active particles on the nature of effective interactions between passive ones.

Collective Motion and Pattern Formation in Phase-Synchronizing Active Fluids

Many active particles, such as swimming micro-organisms or motor proteins, do work on their environment by going though a periodic sequence of shapes. Interactions between particles can lead to synchronization of their duty cycles. Here, we study the collective dynamics of a suspension of active particles coupled through hydrodynamics. We find that at high enough density the system transitions to a state of collective motion by a mechanism that is distinct from other instabilities in active matter systems. Second, we demonstrate that the emergent nonequilibrium states feature stationary chimera patterns in which synchronized and phase-isotropic regions coexist. Third, we show that in confinement, oscillatory flows and robust unidirectional pumping states exist, and can be selected by choice of alignment boundary conditions. These results point toward a new route to collective motion and pattern formation and could guide the design of new active materials.

Confined active matter in external fields.

We analyze a dilute suspension of active particles confined between walls and subjected to fields that can modulate particle speed as well as orientation. Generally, the particle distribution is different in the bulk compared to near the walls. In the bulk, particles tend to accumulate in the regions of low speed, but in the presence of an orienting field normal to the walls, particles rotate to align with the field and accumulate in the field direction. At the walls, particles tend to accumulate pointing into the walls and thereby exert pressure on walls. But the presence of strong orienting fields can cause the particles to reorient away from the walls, and hence shows a possible mechanism for preventing contamination of surfaces. The pressure at the walls depends on the wall separation and the field strengths. This work demonstrates how multiple fields with different functionalities can be used to control active matter under confinement.

Active Stokesian dynamics

Since its development, Stokesian dynamics has been a leading approach for the dynamic simulation of suspensions of particles at arbitrary concentrations with full hydrodynamic interactions. Although developed originally for the simulation of passive particle suspensions, the Stokesian dynamics framework is equally well suited to the analysis and dynamic simulation of suspensions of active particles, as we elucidate here. We show how the reciprocal theorem can be used to formulate the exact dynamics for a suspension of arbitrary active particles, and then show how the Stokesian dynamics method provides a rigorous way to approximate and compute the dynamics of dense active suspensions where many-body hydrodynamic interactions are important.

Nonequilibrium dynamical structure factor of a dilute suspension of active particles in a viscoelastic fluid.

In this work we investigate the dynamics of the number-density fluctuations of a dilute suspension of active particles in a linear viscoelastic fluid. We propose a model for the frequency-dependent diffusion coefficient of the active particles which captures the effect of rotational diffusion on the persistence of their self-propelled motion and the viscoelasticity of the medium. Using fluctuating hydrodynamics, the linearized equationsfor the active suspension are derived, from which we calculate its dynamic structure factor and the corresponding intermediate scattering function. For a Maxwell-type rheological model, we find an intricate dependence of these functions on the parameters that characterize the viscoelasticity of the solvent and the activity of the particles, which can significantly deviate from those of an inert suspension of passive particles and of an active suspension in a Newtonian solvent. In particular, in some regions of the parameter space we uncover the emergence of oscillations in the intermediate scattering function at certain wave numbers which represent the hallmark of the nonequilibrium particle activity in the dynamical structure of the suspension and also encode the viscoelastic properties of the medium.

Stokes traction on an active particle.

The mechanics and statistical mechanics of a suspension of active particles are determined by the traction (force per unit area) on their surfaces. Here we present an exact solution of the direct boundary integral equationfor the traction on a spherical active particle in an imposed slow viscous flow. Both single- and double-layer integral operators can be simultaneously diagonalized in a basis of irreducible tensorial spherical harmonics and the solution, thus, can be presented as an infinite number of linear relations between the harmonic coefficients of the traction and the velocity at the boundary of the particle. These generalize Stokes laws for the force and torque. Using these relations we obtain simple expressions for physically relevant quantities such as the symmetric-irreducible dipole acting on, or the power dissipated by, an active particle in an arbitrary imposed flow. We further present an explicit expression for the variance of the Brownian contributions to the traction on an active colloid in a thermally fluctuating fluid.

A fast Chebyshev method for the Bingham closure with application to active nematic suspensions

Continuum kinetic theories provide an important tool for the analysis and simulation of particle suspensions. When those particles are anisotropic, the addition of a particle orientation vector to the kinetic description yields a 2d−1 dimensional theory which becomes intractable to simulate, especially in three dimensions or near states where the particles are highly aligned. Coarse-grained theories that track only moments of the particle distribution functions provide a more efficient simulation framework, but require closure assumptions. For the particular case where the particles are apolar, the Bingham closure has been found to agree well with the underlying kinetic theory; yet the closure is non-trivial to compute, requiring the solution of an often nearly-singular nonlinear equation at every spatial discretization point at every timestep. In this paper, we present a robust, accurate, and efficient numerical scheme for evaluating the Bingham closure, with a controllable error/efficiency tradeoff. To demonstrate the utility of the method, we carry out high-resolution simulations of a coarse-grained continuum model for a suspension of active particles in parameter regimes inaccessible to kinetic theories. Analysis of these simulations reveals that inaccurately computing the closure can act to effectively limit spatial resolution in the coarse-grained fields. Pushing these simulations to the high spatial resolutions enabled by our method reveals a coupling between vorticity and topological defects in the suspension director field, as well as signatures of energy transfer between scales in this active fluid model.

The collective motion of thermophoretic-type active particle suspension under spatial–temporal modulation

The mesoscopic collective behavior of a thermophoretic-type active particle suspension under a spatial–temporal modulated excitation field is experimentally studied. By using a digital light processing chip, a sinusoidal-like spatial–temporal varying laser pattern (intensity wave) is projected on the particle suspension to modulate the particle propulsion strength through the thermophoretic effect and to exert spatial confinement through the optical trapping effect. For static and slow (wave speed ≪ particle propulsion speed) modulations, in contrast to the passive particles trapped around the wave crest, the self-propulsion strength splits the particle distribution into two branches adjacent to the edges of confinement similar to the bacteria system, and the profile of particle distribution moves coherently with the modulation wave. Once the wave speed increases to the order of the particle propulsion speed, the splitting of particle distribution disappears. Furthermore, it is remarkable that the forward propagating modulation-induced certain fraction of backward streaming particles are observed. This is a generic behavior of a self-propelling active particle suspension, which is not found in the bacteria system. This finding should be useful for particle manipulation at the mesoscopic scale.

Mesoscopic clustering behavior of thermophoretic-type active particle suspension under quasi-one-dimensional microconfinement.

We experimentally investigate the mesoscopic clustering behavior of thermophoretic-type active particle suspension under quasi-one-dimensional spatial confinement (high aspect ratio microchannel). The microchannel enhances the viscous dissipation to operate the system in subpropulsion regime. We find that, in the subpropulsion regime, the steady-state configuration of active particle suspension exhibits a transition from homogeneous state to sausagelike clustering bundle located at the channel center, quasiperiodic isolated clusters at the channel center, aperiodic isolated cluster deviated from channel center, and finally to the typical propulsion-induced accumulation around the channel boundary as increasing the excitation laser intensity. The formation of those patterns is under the interplay of outward-pointing mesoscopic scaled thermophoretic force and the applied spatial confinement. The finding of those special patterns can provide some further possibilities of particle manipulation at mesoscopic scale.

Irreversibility and chaos in active particle suspensions

The collective behavior of active suspensions of microswimmers immersed in a viscous fluid is investigated through numerical studies. It is shown that a bioturbulent state emerges both in suspensions of pushers and of pullers. Which conditions are needed to trigger such phenomenology and what mechanisms underlie such phenomena are discussed. An investigation into whether the difference in puller and pusher dynamics is due to a spontaneous breaking of the hydrodynamics time-reversal symmetry is presented, and the mechanisms underlying such broken symmetry in biological swimmers are examined.

Effective Langevin equations for a polar tracer in an active bath

We study the motion of a polar tracer, having a concave surface, immersed in a two-dimensional suspension of active particles. Using Brownian dynamics simulations, we measure the distributions and auto-correlation functions of force and torque exerted by active particles on the tracer. The tracer experiences a finite average force along its polar axis, while all the correlation functions show exponential decay in time. Using these insights we construct the full coarse-grained Langevin description for tracer position and orientation, where the active particles are subsumed into an effective self-propulsion force and exponentially correlated noise for both translations and rotations. The ensuing mesoscopic dynamics can be described in terms of five dimensionless parameters. We perform a thorough parameter study of the mean squared displacement, which illustrates how the different parameters influence the tracer dynamics, which crosses over from a ballistic to diffusive motion. We also demonstrate that the distribution of tracer displacements evolves from a non-Gaussian shape at early stages to a Gaussian behavior for sufficiently long times. Finally, for a given set of microscopic parameters, we establish a procedure to estimate the matching parameters of our effective model, and show that the resulting dynamics is in a very good quantitative agreement with the one obtained in Brownian dynamics simulations.

Collective forces in scalar active matter.

Large-scale collective behavior in suspensions of active particles can be understood from the balance of statistical forces emerging beyond the direct microscopic particle interactions. Here we review some aspects of the collective forces that can arise in suspensions of self-propelled active Brownian particles: wall forces under confinement, interfacial forces, and forces on immersed bodies mediated by the suspension. Even for non-aligning active particles, these forces are intimately related to a non-uniform polarization of particle orientations induced by walls and bodies, or inhomogeneous density profiles. We conclude by pointing out future directions and promising areas for the application of collective forces in synthetic active matter, as well as their role in living active matter.

The mesoscopic collective motion of self-propelling active particle suspension confined in two-dimensional micro-channel

The mesoscopic collective motion of self-propelling active particle suspension confined in high aspect ratio two-dimensional micro-channel is numerically studied through coupled equation by considering background thermal fluctuation, inter-particle interaction, self-propulsion and micro-channel confinement. Both the self-propulsion and micro-channel confinement are the factors driving the system away from equilibrium and sustaining heterogeneous motion. In such system, the propulsion induced particle accumulation around the channel walls is a universal phenomenon with spatial heterogeneity, where large fraction of particles are caged inside the accumulated cluster with local oscillation coexisting with few fast propelling particles in the center region. Although the formation mechanism of the induced accumulation is well studied, post the cluster formation, how the cluster evolves and its dynamical properties is rarely discussed. Based on the merits of equation, the dynamical evolution of induced accumulation is revealed by particle trajectories. It is found that the induced accumulation can be dissociated through the slow re-orientation process of few jammed particles. By using the idea of force chain network, how the transverse confinement couples the transverse displacement with the longitudinal displacement is evidenced. It is further verified by the statistical measurement of correlation probability between transverse and longitudinal displacements. The suppressed displacements in both directions is the origin leading to the slow dynamics of cluster evolution. Temporally, within the orientational relaxation time, this system exhibits non-trivial anomalous diffusion under the competition between the counter effects of self-propulsion (enhanced diffusion) and micro-channel confinement (suppressed diffusion). Additionally, by considering the orientational coupling, the deep hysteresis of accumulation has been found even for very weak orientational coupling strength.

Dispersion of active particles in confined unidirectional flows

Transport of micro-organisms in confined flows can be characterized by a one-dimensional overall dispersion mechanism, of importance to various biotechnological applications. Based on Brenner’s generalized Taylor dispersion theory, an overall dispersion model is analytically studied in the present work for a dilute suspension of active particles in confined unidirectional flows. With the confined section of the channel and the swimming orientation space taken together as the local space and the longitudinal coordinate standing for the one-dimensional global space, this model is analytically accurate and possessed of wide adaptability in terms of the swimming Péclet number. The Robin boundary condition is introduced to account for wall accumulation of active particles, and compared with a typical reflection boundary condition. Complications associated with the boundary conditions for analytical derivation are removed respectively by a decomposition of the distribution function and an extension of the flow field. Interesting solutions are concretely found and intensively illustrated. Detailed case studies on the transport of spherical and rod-like particles to illustrate the dispersion mechanism are presented with respect to a Couette flow and a plane Poiseuille flow. Associated with the local distribution of particles, extensive descriptions are given for the dynamical system behaviours such as accumulation near both stable points/lines and boundaries, symmetric polarization structure, closed orbits, trapping effect, nematic alignments and bimodalization of swimming direction. For spherical particles, the accumulation is shown leading to a reduction of the overall dispersivity in both of the flows, while for rod-like active particles in the Couette flow, the accumulation can result in an enhancement of dispersion, due to the nematic alignments of particles towards streamlines.

Charged Nanoparticles Quench the Propulsion of Active Janus Colloids.

Active colloidal particles regularly interact with surfaces in applications ranging from microfluidics to sensing. Recent work has revealed the complex nature of these surface interactions for active particles. Herein, we summarize experiments and simulations that show the impact of charged nanoparticles on the propulsion of an active colloid near a boundary. Adding charged nanoparticles not only decreased the average separation distance of a passive colloid because of depletion attraction as expected but also decreased the apparent propulsion of a Janus colloid to near zero. Complementary agent-based simulations considering the impact of hydrodynamics for active Janus colloids were conducted in the range of separation distances inferred from experiment. These simulations showed that propulsion speed decreased monotonically with decreasing average separation distance. Although the trend found in experiments and simulations was in qualitative agreement, there was still a significant difference in the magnitude of speed reduction. The quantitative difference was attributed to the influence of charged nanoparticles on the conductivity of the active particle suspension. Follow-up experiments delineating the impact of depletion and conductivity showed that both contribute to the reduction of speed for an active Janus particle. The experimental and simulated data suggests that it is necessary to consider the synergistic effects between various mechanisms influencing interactions experienced by an active particle near a boundary.

Interphases in Electroactive Suspension Systems: Where Chemistry Meets Mesoscale Physics

AbstractInvited for this month's cover picture the group of Prof. Alejandro A. Franco from LRCS, Amiens, France. The cover picture shows a semisolid redox flow battery set against a background depicting the degree of complexity within the system. Read the full text of the review at 10.1002/batt.201800152.

Interphases in Electroactive Suspension Systems: Where Chemistry Meets Mesoscale Physics

AbstractSemi‐solid redox flow batteries (SSRFBs) consist of electrochemically active particle suspensions as electrodes and can potentially be applied to large scale energy storage. Invented just a decade ago, these batteries already face dwindling commercial value as they can be too complex to study systematically. This review illustrates the depth and width of the state of the art of knowledge that needs to be taken into account. Additionally, this work shows how SSRFBs are an embodiment of complex systems. Conventional theoretical paradigms, experimental tools, and modeling methods generally reduce the size of the problem to solve it. However, this is nearly impossible for highly complex systems with interdependent parameter relationships. This review shows how rheology plays a very significant role in impacting electrochemistry. It concluds that the fastest way to optimize SSRFBs is by obtaining as many experimentally observable parameters as possible using advanced simultaneous techniques, followed by incorporation of this multidisciplinary data into a unified theoretical framework.

Irreversibility in Active Matter Systems: Fluctuation Theorem and Mutual Information

We consider a Brownian particle which, in addition to being in contact with a thermal bath, is driven by fluctuating forces which stem from active processes in the system, such as self-propulsion or collisions with other active particles. These active fluctuations do not fulfill a fluctuation-dissipation relation and therefore play the role of a non-equilibrium environment, which keeps the system permanently out of thermal equilibrium even in the absence of external forces. We investigate how the out-of-equilibrium character of the active matter system and the associated irreversibility is reflected in the trajectories of the Brownian particle. Specifically, we analyze the log-ratio of path probabilities for observing a certain particle trajectory forward in time versus observing its time-reversed twin trajectory. For passive Brownian motion, it is well-known that this path probability ratio quantifies irreversibility in terms of entropy production. For active Brownian motion, we show that in addition to the usual entropy produced in the thermal environment the path probability ratio contains a contribution to irreversibility from mutual information production between the particle trajectory and the history of the non-equilibrium environment. The resulting irreversibility measure fulfills an integral fluctuation theorem and a second-law like relation. When deriving and discussing these relations, we keep in mind that the active fluctuations can occur either due to a suspension of active particles pushing around a passive colloid or due to active self-propulsion of the particle itself; we point out the similarities and differences between these two situations. We obtain explicit expressions for active fluctuations modeled by an Ornstein-Uhlenbeck process. Finally, we illustrate our general results by analyzing a Brownian particle which is trapped in a static or moving harmonic potential.