Pair Interaction between Two Catalytically Active Colloids.

Due to the intrinsically complex non-equilibrium behavior of the constituents of active matter systems, a comprehensive understanding of their collective properties is a challenge that requires systematic bottom-up characterization of the individual components and their interactions. For self-propelled particles, intrinsic complexity stems from the fact that the polar nature of the colloids necessitates that the interactions depend on positions and orientations of the particles, leading to a 2d - 1 dimensional configuration space for each particle, in d dimensions. Moreover, the interactions between such non-equilibrium colloids are generically non-reciprocal, which makes the characterization even more complex. Therefore, derivation of generic rules that enable us to predict the outcomes of individual encounters as well as the ensuing collective behavior will be an important step forward. While significant advances have been made on the theoretical front, such systematic experimental characterizations using simple artificial systems with measurable parameters are scarce. Here, two different contrasting types of colloidal microswimmers are studied, which move in opposite directions and show distinctly different interactions. To facilitate the extraction of parameters, an experimental platform is introduced in which these parameters are confined on a 1D track. Furthermore, a theoretical model for interparticle interactions near a substrate is developed, including both phoretic and hydrodynamic effects, which reproduces their behavior. For subsequent validation, the degrees of freedom are increased to 2D motion and resulting trajectories are predicted, finding remarkable agreement. These results may prove useful in characterizing the overall alignment behavior of interacting self-propelling active swimmer and may find direct applications in guiding the design of active-matter systems involving phoretic and hydrodynamic interactions.

Towards an analytical description of active microswimmers in clean and in surfactant-covered drops.

Geometric confinements are frequently encountered in the biological world and strongly affect the stability, topology, and transport properties of active suspensions in viscous flow. Based on a far-field analytical model, the low-Reynolds-number locomotion of a self-propelled microswimmer moving inside a clean viscous drop or a drop covered with a homogeneously distributed surfactant, is theoretically examined. The interfacial viscous stresses induced by the surfactant are described by the well-established Boussinesq-Scriven constitutive rheological model. Moreover, the active agent is represented by a force dipole and the resulting fluid-mediated hydrodynamic couplings between the swimmer and the confining drop are investigated. We find that the presence of the surfactant significantly alters the dynamics of the encapsulated swimmer by enhancing its reorientation. Exact solutions for the velocity images for the Stokeslet and dipolar flow singularities inside the drop are introduced and expressed in terms of infinite series of harmonic components. Our results offer useful insights into guiding principles for the control of confined active matter systems and support the objective of utilizing synthetic microswimmers to drive drops for targeted drug delivery applications.

Creeping motion of a solid particle inside a spherical elastic cavity: II. Asymmetric motion.

An analytical method is proposed for computing the low-Reynolds-number hydrodynamic mobility function of a small colloidal particle asymmetrically moving inside a large spherical elastic cavity, the membrane of which is endowed with resistance toward shear and bending. In conjunction with the results obtained in the first part (A. Daddi-Moussa-Ider, H. Löwen, S. Gekle, Eur. Phys. J. E 41, 104 (2018)), in which the axisymmetric motion normal to the surface of an elastic cavity is investigated, the general motion for an arbitrary force direction can now be addressed. The elastohydrodynamic problem is formulated and solved using the classic method of images through expressing the hydrodynamic flow fields as a multipole expansion involving higher-order derivatives of the free-space Green's function. In the quasi-steady limit, we demonstrate that the particle self-mobility function of a particle moving tangent to the surface of the cavity is larger than that predicted inside a rigid stationary cavity of equal size. This difference is justified by the fact that a stationary rigid cavity introduces additional hindrance to the translational motion of the encapsulated particle, resulting in a reduction of its hydrodynamic mobility. Furthermore, the motion of the cavity is investigated, revealing that the translational pair (composite) mobility, which linearly couples the velocity of the elastic cavity to the force exerted on the solid particle, is solely determined by membrane shear properties. Our analytical predictions are favorably compared with fully-resolved computer simulations based on a completed-double-layer boundary integral method.

Membrane penetration and trapping of an active particle.

The interaction between nano- or micro-sized particles and cell membranes is of crucial importance in many biological and biomedical applications such as drug and gene delivery to cells and tissues. During their cellular uptake, the particles can pass through cell membranes via passive endocytosis or by active penetration to reach a target cellular compartment or organelle. In this manuscript, we develop a simple model to describe the interaction of a self-driven spherical particle (moving through an effective constant active force) with a minimal membrane system, allowing for both penetration and trapping. We numerically calculate the state diagram of this system, the membrane shape, and its dynamics. In this context, we show that the active particle may either get trapped near the membrane or penetrate through it, where the membrane can either be permanently destroyed or recover its initial shape by self-healing. Additionally, we systematically derive a continuum description allowing us to accurately predict most of our results analytically. This analytical theory helps in identifying the generic aspects of our model, suggesting that most of its ingredients should apply to a broad range of membranes, from simple model systems composed of magnetic microparticles to lipid bilayers. Our results might be useful to predict the mechanical properties of synthetic minimal membranes.

Brownian motion near an elastic cell membrane: A theoretical study.

Elastic confinements are an important component of many biological systems and dictate the transport properties of suspended particles under flow. In this paper, we review the Brownian motion of a particle moving in the vicinity of a living cell whose membrane is endowed with a resistance towards shear and bending. The analytical calculations proceed through the computation of the frequency-dependent mobility functions and the application of the fluctuation-dissipation theorem. Elastic interfaces endow the system with memory effects that lead to a long-lived anomalous subdiffusive regime of nearby particles. In the steady limit, the diffusional behavior approaches that near a no-slip hard wall. The analytical predictions are validated and supplemented with boundary-integral simulations.

Creeping motion of a solid particle inside a spherical elastic cavity⋆.

On the basis of the linear hydrodynamic equations, we present an analytical theory for the low-Reynolds-number motion of a solid particle moving inside a larger spherical elastic cavity which can be seen as a model system for a fluid vesicle. In the particular situation where the particle is concentric with the cavity, we use the stream function technique to find exact analytical solutions of the fluid motion equations on both sides of the elastic cavity. In this particular situation, we find that the solution of the hydrodynamic equations is solely determined by membrane shear properties and that bending does not play a role. For an arbitrary position of the solid particle within the spherical cavity, we employ the image solution technique to compute the axisymmetric flow field induced by a point force (Stokeslet). We then obtain analytical expressions of the leading-order mobility function describing the fluid-mediated hydrodynamic interactions between the particle and the confining elastic cavity. In the quasi-steady limit of vanishing frequency, we find that the particle self-mobility function is higher than that predicted inside a rigid no-slip cavity. Considering the cavity motion, we find that the pair-mobility function is determined only by membrane shear properties. Our analytical predictions are supplemented and validated by fully resolved boundary integral simulations where a very good agreement is obtained over the whole range of applied forcing frequencies.

Swimming trajectories of a three-sphere microswimmer near a wall.

The hydrodynamic flow field generated by self-propelled active particles and swimming microorganisms is strongly altered by the presence of nearby boundaries in a viscous flow. Using a simple model three-linked sphere swimmer, we show that the swimming trajectories near a no-slip wall reveal various scenarios of motion depending on the initial orientation and the distance separating the swimmer from the wall. We find that the swimmer can either be trapped by the wall, completely escape, or perform an oscillatory gliding motion at a constant mean height above the wall. Using a far-field approximation, we find that, at leading order, the wall-induced correction has a source-dipolar or quadrupolar flow structure where the translational and angular velocities of the swimmer decay as inverse third and fourth powers with distance from the wall, respectively. The resulting equations of motion for the trajectories and the relevant order parameters fully characterize the transition between the states and allow for an accurate description of the swimming behavior near a wall. We demonstrate that the transition between the trapping and oscillatory gliding states is first order discontinuous, whereas the transition between the trapping and escaping states is continuous, characterized by non-trivial scaling exponents of the order parameters. In order to model the circular motion of flagellated bacteria near solid interfaces, we further assume that the spheres can undergo rotational motion around the swimming axis. We show that the general three-dimensional motion can be mapped onto a quasi-two-dimensional representational model by an appropriate redefinition of the order parameters governing the transition between the swimming states.

Hydrodynamic coupling and rotational mobilities near planar elastic membranes.

We study theoretically and numerically, the coupling and rotational hydrodynamic interactions between spherical particles near a planar elastic membrane that exhibits resistance toward shear and bending. Using a combination of the multipole expansion and Faxén's theorems, we express the frequency-dependent hydrodynamic mobility functions as a power series of the ratio of the particle radius to the distance from the membrane for the self mobilities and as a power series of the ratio of the radius to the interparticle distance for the pair mobilities. In the quasi-steady limit of zero frequency, we find that the shear- and bending-related contributions to the particle mobilities may have additive or suppressive effects depending on the membrane properties in addition to the geometric configuration of the interacting particles relative to the confining membrane. To elucidate the effect and role of the change of sign observed in the particle self mobilities and pair mobilities, we consider an example involving a torque-free doublet of counterrotating particles near an elastic membrane. We find that the induced rotation rate of the doublet around its center of mass may differ in magnitude and direction depending on the membrane shear and bending properties. Near a membrane of only energetic resistance toward shear deformation, such as that of a certain type of elastic capsules, the doublet undergoes rotation of the same sense as observed near a no-slip wall. Near a membrane of only energetic resistance toward bending, such as that of a fluid vesicle, we find a reversed sense of rotation. Our analytical predictions are supplemented and compared with fully resolved boundary integral simulations where very good agreement is obtained over the whole range of applied frequencies.

Hydrodynamic interaction between particles near elastic interfaces.

We present an analytical calculation of the hydrodynamic interaction between two spherical particles near an elastic interface such as a cell membrane. The theory predicts the frequency dependent self- and pair-mobilities accounting for the finite particle size up to the 5th order in the ratio between particle diameter and wall distance as well as between diameter and interparticle distance. We find that particle motion towards a membrane with pure bending resistance always leads to mutual repulsion similar as in the well-known case of a hard-wall. In the vicinity of a membrane with shearing resistance, however, we observe an attractive interaction in a certain parameter range which is in contrast to the behavior near a hard wall. This attraction might facilitate surface chemical reactions. Furthermore, we show that there exists a frequency range in which the pair-mobility for perpendicular motion exceeds its bulk value, leading to short-lived superdiffusive behavior. Using the analytical particle mobilities we compute collective and relative diffusion coefficients. The appropriateness of the approximations in our analytical results is demonstrated by corresponding boundary integral simulations which are in excellent agreement with the theoretical predictions.

Internal sites of actuation and activation in thin elastic films and membranes of finite thickness.

Functionalized thin elastic films and membranes frequently feature internal sites of net forces or stresses. These are, for instance, active sites of actuation, or rigid inclusions in a strained membrane that induce counterstress upon externally imposed deformations. We theoretically analyze the geometry of isotropic, flat, thin, linearly elastic films or membranes of finite thickness, laterally extended to infinity. At the mathematical core of such characterizations are the fundamental solutions for localized force and stress singularities associated with corresponding Green's functions. We derive such solutions in three dimensions and place them into the context of previous two-dimensional calculations. To this end, we consider both no-slip and stress-free conditions at the top and/or bottom surfaces. We provide an understanding for why the fully free-standing thin elastic membrane leads to diverging solutions in most geometries and compare these situations to the truly two-dimensional case. A no-slip support of at least one of the surfaces stabilizes the solution, which illustrates that the divergences in the fully free-standing case are connected to global deformations. Within the aforementioned framework, our results are important for associated theoretical characterizations of thin elastic films, whether supported or free-standing, and of membranes subject to internal or external forces or stresses.

Minimum entropy production by microswimmers with internal dissipation.

The energy dissipation and entropy production by self-propelled microswimmers differ profoundly from passive particles pulled by external forces. The difference extends both to the shape of the flow around the swimmer, as well as to the internal dissipation of the propulsion mechanism. Here we derive a general theorem that provides an exact lower bound on the total, external and internal, dissipation by a microswimmer. The problems that can be solved include an active surface-propelled droplet, swimmers with an extended propulsive layer and swimmers with an effective internal dissipation. We apply the theorem to determine the swimmer shapes that minimize the total dissipation while keeping the volume constant. Our results show that the entropy production by active microswimmers is subject to different fundamental limits than the entropy production by externally driven particles.

Microparticle Brownian motion near an air-water interface governed by direction-dependent boundary conditions.

HYPOTHESIS: Although the dynamics of colloids in the vicinity of a solid interface has been widely characterized in the past, experimental studies of Brownian diffusion close to an air-water interface are rare and limited to particle-interface gap distances larger than the particle size. At the still unexplored lower distances, the dynamics is expected to be extremely sensitive to boundary conditions at the air-water interface. There, ad hoc experiments would provide a quantitative validation of predictions. EXPERIMENTS: Using a specially designed dual wave interferometric setup, the 3D dynamics of 9 µm diameter particles at a few hundreds of nanometers from an air-water interface is here measured in thermal equilibrium. FINDINGS: Intriguingly, while the measured dynamics parallel to the interface approaches expected predictions for slip boundary conditions, the Brownian motion normal to the interface is very close to the predictions for no-slip boundary conditions. These puzzling results are rationalized considering current models of incompressible interfacial flow and deepened developing an ad hoc model which considers the contribution of tiny concentrations of surface active particles at the interface. We argue that such condition governs the particle dynamics in a large spectrum of systems ranging from biofilm formation to flotation process.

Frequency-dependent higher-order Stokes singularities near a planar elastic boundary: Implications for the hydrodynamics of an active microswimmer near an elastic interface.

The emerging field of self-driven active particles in fluid environments has recently created significant interest in the biophysics and bioengineering communities owing to their promising future for biomedical and technological applications. These microswimmers move autonomously through aqueous media, where under realistic situations they encounter a plethora of external stimuli and confining surfaces with peculiar elastic properties. Based on a far-field hydrodynamic model, we present an analytical theory to describe the physical interaction and hydrodynamic couplings between a self-propelled active microswimmer and an elastic interface that features resistance toward shear and bending. We model the active agent as a superposition of higher-order Stokes singularities and elucidate the associated translational and rotational velocities induced by the nearby elastic boundary. Our results show that the velocities can be decomposed in shear and bending related contributions which approach the velocities of active agents close to a no-slip rigid wall in the steady limit. The transient dynamics predict that contributions to the velocities of the microswimmer due to bending resistance are generally more pronounced than those due to shear resistance. Bending can enhance (suppress) the velocities resulting from higher-order singularities whereas the shear related contribution decreases (increases) the velocities. Most prominently, we find that near an elastic interface of only energetic resistance toward shear deformation, such as that of an elastic capsule designed for drug delivery, a swimming bacterium undergoes rotation of the same sense as observed near a no-slip wall. In contrast to that, near an interface of only energetic resistance toward bending, such as that of a fluid vesicle or liposome, we find a reversed sense of rotation. Our results provide insight into the control and guidance of artificial and synthetic self-propelling active microswimmers near elastic confinements.

State diagram of a three-sphere microswimmer in a channel.

Geometric confinements are frequently encountered in soft matter systems and in particular significantly alter the dynamics of swimming microorganisms in viscous media. Surface-related effects on the motility of microswimmers can lead to important consequences in a large number of biological systems, such as biofilm formation, bacterial adhesion and microbial activity. On the basis of low-Reynolds-number hydrodynamics, we explore the state diagram of a three-sphere microswimmer under channel confinement in a slit geometry and fully characterize the swimming behavior and trajectories for neutral swimmers, puller- and pusher-type swimmers. While pushers always end up trapped at the channel walls, neutral swimmers and pullers may further perform a gliding motion and maintain a stable navigation along the channel. We find that the resulting dynamical system exhibits a supercritical pitchfork bifurcation in which swimming in the mid-plane becomes unstable beyond a transition channel height while two new stable limit cycles or fixed points that are symmetrically disposed with respect to the channel mid-height emerge. Additionally, we show that an accurate description of the averaged swimming velocity and rotation rate in a channel can be captured analytically using the method of hydrodynamic images, provided that the swimmer size is much smaller than the channel height.

Hydrodynamic mobility of a solid particle near a spherical elastic membrane: Axisymmetric motion.

We use the image solution technique to compute the leading order frequency-dependent self-mobility function of a small solid particle moving perpendicular to the surface of a spherical capsule whose membrane possesses shearing and bending rigidities. Comparing our results with those obtained earlier for an infinitely extended planar elastic membrane, we find that membrane curvature leads to the appearance of a prominent additional peak in the mobility. This peak is attributed to the fact that the shear resistance of the curved membrane involves a contribution from surface-normal displacements, which is not the case for planar membranes. In the vanishing frequency limit, the particle self-mobility near a no-slip hard sphere is recovered only when the membrane possesses a nonvanishing resistance toward shearing. We further investigate capsule motion, finding that the pair-mobility function is solely determined by membrane shearing properties. Our analytical predictions are validated by fully resolved boundary integral simulations where a very good agreement is obtained.

Hydrodynamic mobility of a solid particle near a spherical elastic membrane. II. Asymmetric motion.

In this paper, we derive analytical expressions for the leading-order hydrodynamic mobility of a small solid particle undergoing motion tangential to a nearby large spherical capsule whose membrane possesses resistance toward shearing and bending. Together with the results obtained in the first part [Daddi-Moussa-Ider and Gekle, Phys. Rev. E 95, 013108 (2017)2470-004510.1103/PhysRevE.95.013108], where the axisymmetric motion perpendicular to the capsule membrane is considered, the solution of the general mobility problem is thus determined. We find that shearing resistance induces a low-frequency peak in the particle self-mobility, resulting from the membrane normal displacement in the same way, although less pronounced, to what has been observed for the axisymmetric motion. In the zero-frequency limit, the self-mobility correction near a hard sphere is recovered only if the membrane has a nonvanishing resistance toward shearing. We further compute the in-plane mean-square displacement of a nearby diffusing particle, finding that the membrane induces a long-lasting subdiffusive regime. Considering capsule motion, we find that the correction to the pair-mobility function is solely determined by membrane shearing properties. Our analytical calculations are compared and validated with fully resolved boundary integral simulations where a very good agreement is obtained.

Long-lived anomalous thermal diffusion induced by elastic cell membranes on nearby particles.

The physical approach of a small particle (virus, medical drug) to the cell membrane represents the crucial first step before active internalization and is governed by thermal diffusion. Using a fully analytical theory we show that the stretching and bending of the elastic membrane by the approaching particle induces a memory in the system, which leads to anomalous diffusion, even though the particle is immersed in a purely Newtonian liquid. For typical cell membranes the transient subdiffusive regime extends beyond 10 ms and can enhance residence times and possibly binding rates up to 50%. Our analytical predictions are validated by numerical simulations.