Contact charge electrophoresis (CCEP) uses steady electric fields to drive the continuous, oscillatory motion of conductive particles and droplets between two or more electrodes. These rapid oscillations can be rectified to direct the motion of objects within microfluidic environments using low-power, dc voltage. Here, we compare high precision experimental measurements of CCEP within a microfluidic system to equally detailed theoretical predictions on the motion of a conductive particle between parallel electrodes. We use a simple, capillary microfluidic platform that combines high-speed imaging with precision electrical measurements to enable the synchronized acquisition of both the particle location and the electric current due to particle motion. The experimental results are compared to those of a theoretical model, which relies on a Stokesian dynamics approach to accurately describe both the electrostatic and hydrodynamic problems governing particle motion. We find remarkable agreement between theory and experiment, suggesting that particle motion can be accurately captured by a combination of classical electrostatics and low-Reynolds number hydrodynamics. Building on this agreement, we offer new insight into the charge transfer process that occurs when the particle nears contact with an electrode surface. In particular, we find that the particle does not make mechanical contact with the electrode but rather that charge transfer occurs at finite surface separations of >0.1 μm by means of an electric discharge through a thin lubricating film. We discuss the implications of these findings on the charging of the particle and its subsequent dynamics.
We investigate the self-assembly of amphiphilic nanoparticles (NPs) functionalized with mixed monolayers of hydrophobic and hydrophilic ligands in water. Unlike typical amphiphilic particles with "fixed" surface chemistries, the ligands used here are not bound irreversibly but can rearrange dynamically on the particles' surface during their assembly from solution. Depending on the assembly conditions, these adaptive amphiphiles form compact micellar clusters or extended chain-like assemblies in aqueous solution. By controlling the amount of hydrophobic ligands on the particles' surface, the average number of nearest neighbors--that is, the preferred coordination number--can be varied systematically from ∼ 1 (dimers) to ∼ 2 (linear chains) to ∼ 3 (extended clusters). To explain these experimental findings, we present an assembly mechanism in which hydrophobic ligands organize dynamically to form discrete patches between proximal NPs to minimize contact with their aqueous surroundings. Monte Carlo simulations incorporating these adaptive hydrophobic interactions reproduce the three-dimensional assemblies observed in experiment. These results suggest a general strategy based on reconfigurable "sticky" patches that may allow for tunable control over particle coordination number within self-assembled structures.
Small autonomous machines like biological cells or soft robots can convert energy input into control of function and form. It is desired that this behavior emerges spontaneously and can be easily switched over time. For this purpose we introduce an active matter system that is loosely inspired by biology and which we term an active colloidal cell. The active colloidal cell consists of a boundary and a fluid interior, both of which are built from identical rotating spinners whose activity creates convective flows. Similarly to biological cell motility, which is driven by cytoskeletal components spread throughout the entire volume of the cell, active colloidal cells are characterized by highly distributed energy conversion. We demonstrate that we can control the shape of the active colloidal cell and drive compartmentalization by varying the details of the boundary (hard vs. flexible) and the character of the spinners (passive vs. active). We report buckling of the boundary controlled by the pattern of boundary activity, as well as formation of core-shell and inverted Janus phase-separated configurations within the active cell interior. As the cell size is increased, the inverted Janus configuration spontaneously breaks its mirror symmetry. The result is a bubble-crescent configuration, which alternates between two degenerate states over time and exhibits collective migration of the fluid along the boundary. Our results are obtained using microscopic, non-momentum-conserving Langevin dynamics simulations and verified via a phase-field continuum model coupled to a Navier-Stokes equation.active matter | emergent pattern | confinement | colloids A ctive matter describes particulate systems with the characteristic that each "particle" (agent) converts energy into motion (1, 2). Active matter covers a range of length scales that include molecular motors in the cytoskeleton (3-5), swimming bacteria (6-8), driven colloids (9, 10), flocks of birds and fish (11)(12)(13)(14), and people and vehicles in motion (15). Over the last decade, studies of active matter have demonstrated behavior not seen in equilibrium systems, including giant number fluctuations (16, 17), emergent attraction and superdiffusion (18)(19)(20), clustering (21, 22), swarming (23-27), and self-assembled motifs (28, 29). These systems provide interesting theoretical and engineering challenges as well as opportunities to explore and target novel behaviors that proceed outside of thermodynamic equilibrium.Of particular interest are systems found in nature or inspired by natural phenomena. Biological systems usually operate in confined regions of space--think of intracellular space, interfaces and membranes, and the crowding of cells near surfaces. The role of hydrodynamics in confinement has been studied for biological swimmers, such as bacteria and sperm, showing accumulation at the walls (30-32) and upstream swimming along surfaces (33) or in a spiral vortex (34-36). Attraction to walls has also been reported in the absence of hydrodynamics for disks (37...
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