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Joakim Stenhammar

Publications and source records attributed to Joakim Stenhammar.

30 records · Page 2Linked to original sources

Reversible Formation of Thermoresponsive Binary Particle Gels with Tunable Structural and Mechanical Properties

We investigate the collective behavior of suspended thermoresponsive microgels, that expel solvent and subsequently decrease in size upon heating. Using a binary mixture of differently thermoresponsive microgels, we demonstrate how distinctly different gel structures form, depending on the heating profile used. Confocal laser scanning microscopy (CLSM) imaging shows that slow heating ramps yield a core-shell network through sequential gelation, while fast heating ramps yield a random binary network through homo-gelation. Here, secondary particles are shown to aggregate in a monolayer fashion upon the first gel, which can be qualitatively reproduced through Brownian dynamics simulations using a model based on a temperature-dependent interaction potential incorporating steric repulsion and van der Waals attraction. Through oscillatory rheology it is shown that secondary microgel deposition enhances the structural integrity of the previously formed single species gel, and the final structure exhibits higher elastic and loss moduli than its compositionally identical homo-gelled counterpart. Furthermore, we demonstrate that aging processes in the scaffold before secondary microgel deposition govern the final structural properties of the bigel, which allows a detailed control over these properties. Our results thus demonstrate how the temperature profile can be used to finely control the structural and mechanical properties of these highly tunable materials.

cond-mat.soft↗

Generalized thermodynamics of Motility-Induced Phase Separation: Phase equilibria, Laplace pressure, and change of ensembles

Motility-induced phase separation (MIPS) leads to cohesive active matter in the absence of cohesive forces. We present, extend and illustrate a recent generalized thermodynamic formalism which accounts for its binodal curve. Using this formalism, we identify both a generalized surface tension, that controls finite-size corrections to coexisting densities, and generalized forces, that can be used to construct new thermodynamic ensembles. Our framework is based on a nonequilibrium generalization of the Cahn-Hilliard equation and we discuss its application to active particles interacting either via quorum-sensing interactions or directly through pairwise forces.

cond-mat.stat-mech↗

Generalized Thermodynamics of Phase Equilibria in Scalar Active Matter

Motility-induced phase separation (MIPS) arises generically in fluids of self-propelled particles when interactions lead to a kinetic slowdown at high densities. Starting from a continuum description of scalar active matter, akin to a generalized Cahn-Hilliard equation, we give a general prescription for the mean densities of coexisting phases in flux-free steady states that amounts, at a hydrodynamics scale, to extremizing an effective free energy. We illustrate our approach on two well-known models: self-propelled particles interacting either through a density-dependent propulsion speed or via direct pairwise forces. Our theory accounts quantitatively for their phase diagrams, providing a unified description of MIPS.

cond-mat.stat-mech↗

Directed Self-Assembly of Polarizable Ellipsoids in an External Electric Field

The interplay between shape anisotropy and directed long-range interactions enables the self-assembly of complex colloidal structures. As a recent highlight, ellipsoidal particles polarized in an external electric field were observed to associate into well-defined tubular structures. In this study, we investigate systematically such directed self-assembly using Monte Carlo simulations of a two-point-charge model of polarizable prolate ellipsoids. In spite of its simplicity and computational efficiency, we demonstrate that the model is capable of capturing the complex structures observed in experiments on ellipsoidal colloids at low volume fractions. We show that, at sufficiently high electric field strength, the anisotropy in shape and electrostatic interactions causes a transition from 3-dimensional crystal structures observed at low aspect ratios to 2-dimensional sheets and tubes at higher aspect ratios. Our work thus illustrates the rich self-assembly behavior accessible when exploiting the interplay between competing long- and short-range anisotropic interactions in colloidal systems.

cond-mat.soft↗

The role of correlations in the collective behaviour of microswimmer suspensions

In this Letter, we study the collective behaviour of a large number of self-propelled microswimmers immersed in a fluid. Using unprecedently large-scale lattice Boltzmann simulations, we reproduce the transition to bacterial turbulence. We show that, even well below the transition, swimmers move in a correlated fashion that cannot be described by a mean-field approach. We develop a novel kinetic theory that captures these correlations and is non-perturbative in the swimmer density. To provide an experimentally accessible measure of correlations, we calculate the diffusivity of passive tracers and reveal its non-trivial density dependence. The theory is in quantitative agreement with the lattice Boltzmann simulations and captures the asymmetry between pusher and puller swimmers below the transition to turbulence.

cond-mat.soft↗

Stirring by Periodic Arrays of Microswimmers

The interaction between swimming microorganisms or artificial self-propelled colloids and passive (tracer) particles in a fluid leads to enhanced diffusion of the tracers. This enhancement has attracted strong interest, as it could lead to new strategies to tackle the difficult problem of mixing on a microfluidic scale. Most of the theoretical work on this topic has focused on hydrodynamic interactions between the tracers and swimmers in a bulk fluid. However, in simulations, periodic boundary conditions (PBCs) are often imposed on the sample and the fluid. Here, we theoretically analyze the effect of PBCs on the hydrodynamic interactions between tracer particles and microswimmers. We formulate an Ewald sum for the leading-order stresslet singularity produced by a swimmer to probe the effect of PBCs on tracer trajectories. We find that introducing periodicity into the system has a surprisingly significant effect, even for relatively small swimmer-tracer separations. We also find that the bulk limit is only reached for very large system sizes, which are challenging to simulate with most hydrodynamic solvers.

cond-mat.soft↗

Nonequilibrium dynamics of mixtures of active and passive colloidal particles

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 spinodal instability can be of two different types. One type is associated with a stationary bifurcation and occurs also in one-component active systems, whereas the other type is associated with a Hopf bifurcation and can occur only in active-passive mixtures. Remarkably, the Hopf bifurcation leads to moving clusters. This explains recent results from simulations of active-passive particle mixtures, where moving clusters and interfaces that are not seen in the corresponding one-component systems have been observed.

cond-mat.soft↗

Lattice-Boltzmann Simulations of Microswimmer-Tracer Interactions

Hydrodynamic interactions in systems comprised of self-propelled particles, such as swimming microorganisms, and passive tracers have a significant impact on the tracer dynamics compared to the equivalent "dry" sample. However, such interactions are often difficult to take into account in simulations due to their computational cost. Here, we perform a systematic investigation of swimmer-tracer interaction using an efficient force/counter-force based lattice-Boltzmann (LB) algorithm [J. de Graaf~\textit{et al.}, J. Chem. Phys.~\textbf{144}, 134106 (2016)] in order to validate its ability to capture the relevant low-Reynolds-number physics. We show that the LB algorithm reproduces far-field theoretical results well, both in a system with periodic boundary conditions and in a spherical cavity with no-slip walls, for which we derive expressions here. The force-lattice coupling of the LB algorithm leads to a "smearing out" of the flow field, which strongly perturbs the tracer trajectories at close swimmer-tracer separations, and we analyze how this effect can be accurately captured using a simple renormalized hydrodynamic theory. Finally, we show that care must be taken when using LB algorithms to simulate systems of self-propelled particles, since its finite momentum transport time can lead to significant deviations from theoretical predictions based on Stokes flow. These insights should prove relevant to the future study of large-scale microswimmer suspensions using these methods.

physics.flu-dyn↗

Activity-induced phase separation and self-assembly in mixtures of active and passive particles

We investigate the phase behavior and kinetics of a monodisperse mixture of active (\textit{i.e.}, self-propelled) and passive isometric Brownian particles through Brownian dynamics simulations and theory. As in a purely active system, motility of the active component triggers phase separation into a dense and a dilute phase; in the dense phase we further find active-passive segregation, with "rafts" of passive particles in a "sea" of active particles. We find that phase separation from an initially disordered mixture can occur with as little as 15 percent of the particles being active. Finally, we show that a system prepared in a suitable fully segregated initial state reproducibly self-assembles an active "corona" which triggers crystallization of the passive core by initiating a compression wave. Our findings are relevant to the experimental pursuit of directed self-assembly using active particles.

cond-mat.soft↗

Scalar $ϕ^4$ field theory for active-particle phase separation

Recent theories predict phase separation among orientationally disordered active particles whose propulsion speed decreases rapidly enough with density. Coarse-grained models of this process show time-reversal symmetry (detailed balance) to be restored for uniform states, but broken by gradient terms; hence detailed-balance violation is strongly coupled to interfacial phenomena. To explore the subtle generic physics resulting from such coupling we here introduce `Active Model B'. This is a scalar $ϕ^4$ field theory (or phase-field model) that minimally violates detailed balance via a leading-order square-gradient term. We find that this additional term has modest effects on coarsening dynamics, but alters the static phase diagram by creating a jump in (thermodynamic) pressure across flat interfaces. Both results are surprising, since interfacial phenomena are always strongly implicated in coarsening dynamics but are, in detailed-balance systems, irrelevant for phase equilibria.

cond-mat.soft↗

Phase behaviour of active Brownian particles: The role of dimensionality

Recently, there has been much interest in activity-induced phase separations in concentrated suspensions of "active Brownian particles" (ABPs), self-propelled spherical particles whose direction of motion relaxes through thermal rotational diffusion. To date, almost all these studies have been restricted to 2 dimensions. In this work we study activity-induced phase separation in 3D and compare the results with previous and new 2D simulations. To this end, we performed state-of-the-art Brownian dynamics simulations of up to 40 million ABPs -- such very large system sizes are unavoidable to evade finite size effects in 3D. Our results confirm the picture established for 2D systems in which an activity-induced phase separation occurs, with strong analogies to equilibrium gas-liquid spinodal decomposition, in spite of the purely non-equilibrium nature of the driving force behind the phase separation. However, we also find important differences between the 2D and 3D cases. Firstly, the shape and position of the phase boundaries is markedly different for the two cases. Secondly, for the 3D coarsening kinetics we find that the domain size grows in time according to the classical diffusive $t^{1/3}$ law, in contrast to the nonstandard subdiffusive exponent observed in 2D.

cond-mat.soft↗

A continuum theory of phase separation kinetics for active Brownian particles

Active Brownian particles (ABPs), when subject to purely repulsive interactions, are known to undergo activity-induced phase separation broadly resembling an equilibrium (attraction-induced) gas-liquid coexistence. Here we present an accurate continuum theory for the dynamics of phase-separating ABPs, derived by direct coarse-graining, capturing leading-order density gradient terms alongside an effective bulk free energy. Such gradient terms do not obey detailed balance; yet we find coarsening dynamics closely resembling that of equilibrium phase separation. Our continuum theory is numerically compared to large-scale direct simulations of ABPs and accurately accounts for domain growth kinetics, domain topologies and coexistence densities.

cond-mat.soft↗