Scalable high-throughput microfluidic separation of magnetic microparticles.

Surface-engineered magnetic microparticles are used in chemical and biomedical engineering due to their ease of synthesis, high surface-to-volume ratio, selective binding, and magnetic separation. To separate them from fluid suspensions, existing methods rely on the magnetic force introduced by the local magnetic field gradient. However, this strategy has poor scalability because the magnetic field gradient decreases rapidly as one moves away from the magnets. Here, we present a scalable high-throughput magnetic separation strategy using a rotating permanent magnet and two-dimensional arrays of micromagnets. Under a dynamic magnetic field, nickel micromagnets allow the surrounding magnetic microparticles to self-assemble into large clusters and effectively propel themselves through the flow. The collective speed of the microparticle swarm reaches about two orders of magnitude higher than the gradient-based separation method over a wide range of operating frequencies and distances from a rotating magnet.

Capture and transport of rod-shaped cargo via programmable active particles.

We study the influence of the cargo shape on the capture and transport process of colloidal rods via swarms of active particles using Brownian dynamics simulations. Starting at random initial conditions, active particles that interact via the Lennard-Jones potential and possess a tuneable speed are utilised to capture passive rods inside a hexagonal cage of individually addressable units. By adjusting the velocity of the individual active particles, the rod can then be transported. To guarantee a successful capture process (with a strong localisation), we find that specific geometric and energetic constraints have to be met; i.e., the length of the rod must approximately be in the vicinity of an odd multiple of the lattice constant of the hexagonal cage, and the Lennard-Jones interaction strength must be in the range of [Formula: see text] to [Formula: see text]. If the cargo aspect ratio gets too large, the subsequent transport of successfully captured rods can fail. For systems where transport is possible, an increase in the cargo aspect ratio decreases the achievable transport velocity. Our work shows that the particle shape must be considered while designing interaction rules to accomplish specific tasks via groups of controllable units.

Diffusion coefficients of linear trimer particles.

We study the diffusive behavior of linear trimer particles via numerical calculations. First, we utilize hydrodynamic bead-shell calculations to compute the microscopic diffusion coefficients for different particle aspect ratios. These values are then used to obtain continuous empirical formulas for said coefficients. As an application example for the empirical formulas, we perform Brownian dynamics simulations of monolayers consisting of a linear trimer surrounded by colloidal spheres. Here, we obtain empirical formulas for the corresponding long-time diffusion coefficients of the trimer. By comparing our data for the microscopic and long-time diffusion coefficients with known results for spherocylinders, we find that the diffusive behavior of both particle geometries is approximately identical. Based on this observation, we introduce simplified equations for the microscopic diffusion coefficients that can be used for arbitrary short rods that are spheres at the minimum aspect ratios. The calculated equations for the diffusion coefficients can be applied to various further numerical and experimental studies utilizing linear trimer particles.

Group formation and collective motion of colloidal rods with an activity triggered by visual perception.

We investigate the formation of cohesive groups and the collective diffusion of colloidal spherocylinders with a motility driven by a simple visual perception model. For this, we perform Brownian dynamics simulations without hydrodynamic interactions. The visual perception is based on sight cones attached to the spherocylinders and perception functions quantifying the visual stimuli. If the perception function of a particle reaches a predefined threshold, an active component is added to its motion. We find that, in addition to the opening angle of the cone of sight, the aspect ratio of the particles plays an important role for the formation of cohesive groups. If the elongation of the particles is increased, the maximum angle for which the rods organize themselves into such groups decreases distinctly. After a system forms a cohesive group, it performs a diffusive motion, which can be quantified by an effective diffusion coefficient. For increasing aspect ratios, the spatial expansion of the cohesive groups and the effective diffusion coefficient of the collective motion increase, while the number of active group members decreases. We also find that a larger particle number, a smaller propulsion velocity of the group members, and a smaller threshold for the visual stimulus increase the maximum opening angle for which cohesive groups form. Based on our results, we expect anisotropic particles to be of great relevance for the adjustability of visual perception-dependent motility.

Role of cohesion in the flow of active particles through bottlenecks.

We experimentally and numerically study the flow of programmable active particles (APs) with tunable cohesion strength through geometric constrictions. Similar to purely repulsive granular systems, we observe an exponential distribution of burst sizes and power-law-distributed clogging durations. Upon increasing cohesion between APs, we find a rather abrupt transition from an arch-dominated clogging regime to a cohesion-dominated regime where droplets form at the aperture of the bottleneck. In the arch-dominated regime the flow-rate only weakly depends on the cohesion strength. This suggests that cohesion must not necessarily decrease the group's efficiency passing through geometric constrictions or pores. Such behavior is explained by "slippery" particle bonds which avoids the formation of a rigid particle network and thus prevents clogging. Overall, our results confirm the general applicability of the statistical framework of intermittent flow through bottlenecks developed for granular materials also in case of active microswimmers whose behavior is more complex than that of Brownian particles but which mimic the behavior of living systems.

Microscopic diffusion coefficients of dumbbell- and spherocylinder-shaped colloids and their application in simulations of crowded monolayers.

We explore the diffusion properties of colloidal particles with dumbbell and spherocylinder shapes using a hydrodynamic bead-shell approach and additional Brownian dynamics (BD) simulations. By applying the bead-shell method, we determine empirical formulas for the microscopic diffusion coefficients. A comparison of these formulas and established experimental and theoretical results shows remarkable agreement. For example, the maximum relative discrepancy found for dumbbells is less than 5%. As an application example of the empirical formulas, we perform two-dimensional (2D) BD simulations based on a single dumbbell or spherocylinder in a suspension of spheres and calculate the resulting effective long-time diffusion coefficients. The performed BD simulations can be compared to quasi-2D systems such as colloids confined at the interface of two fluids. We find that the effective diffusion coefficient of translation mostly depends on the sphere area fraction ϕ, while the effective diffusion coefficient of rotation is influenced by the aspect ratio and ϕ. Furthermore, the effective rotational diffusion constant seems to depend on the particle shape with the corresponding implementation of the interactions. In the resolution limit of our methods, the shape-dependent differences of the microscopic diffusion coefficients and the long-time diffusion constant of translation are negligible in the first approximation. The determined empirical formulas for the microscopic diffusion coefficients add to the knowledge of the diffusion of anisotropic particles, and they can be used in countless future studies.

Phase behaviour in 2D assemblies of dumbbell-shaped colloids generated under geometrical confinement.

The structure formation and the phase behaviour of monolayers of dumbbell-shaped colloids are explored. For this, we conduct Langmuir-Blodgett experiments at the air/water interface and conventional Brownian dynamic simulations without hydrodynamic interactions. Using Voronoi tessellations and the probability density of the corresponding shape factor of the Voronoi cells p(ζ), the influence of the area fraction φ on the structure of the monolayers is investigated. An increase of the area fraction leads to a higher percentage of domains containing particles with six nearest neighbours and a sharper progression of p(ζ). Especially in dense systems, these domains can consist of aligned particles with uniform Voronoi cells. Thus, the increase of φ enhances the order of the monolayers. Simulations show that a sufficient enhancement of φ also impacts the pair correlation function which develops a substructure in its first maxima. Furthermore, we find that reducing the barrier speed in the Langmuir-Blodgett experiments enhances the final area fraction for a given target surface pressure which, in turn, also increases the percentage of particles with six nearest neighbours and sharpens the progression of p(ζ). Overall, the experiments and simulations show a remarkable qualitative agreement which indicates a versatile way of characterising colloidal monolayers by Brownian dynamics simulations. This opens up perspectives for application to a broad range of nanoparticle-based thin film coatings and devices.

Dynamic ordering of driven spherocylinders in a nonequilibrium suspension of small colloidal spheres.

The ordering effects of driven spherocylinder-shaped rods in a colloidal suspension of small spheres confined to a two-dimensional channel geometry are observed via Brownian dynamics simulations without hydrodynamics. To describe the ordering, an order parameter and an expression for a potential of mean force of an equivalent equilibrium system are defined and analyzed. By varying the application point of the external force along the rods and thus the resulting lever, a transition from a preferred orientation parallel to the direction of the force to a preferred orientation perpendicular to the direction of the force was observed. It is shown that this effect can only be found if the spheres and multiple rods are present. Furthermore, a dependency of the order parameter on the absolute value of the force was discovered. The analysis of the potential of mean force further indicates a transition between two different phases of mean orientation. An observation of the flow equilibrium mean velocity in channel direction led to a s-shaped progression regarding the lever dependency, also marking a transition between two states linked to the mean orientation of the rods. A finite size analysis was conducted. Its results indicate that the transition between the two orientation states is a general phenomenon of the observed rod-sphere mixture.