Ran Niu

Self-Assembly of Colloidal Molecules due to Self-Generated Flow

The emergence of structure through aggregation is a fascinating topic and of both fundamental and practical interest. Here we demonstrate that self-generated solvent flow can be used to generate long-range attractions on the colloidal scale, with subpiconewton forces extending into the millimeter range. We observe a rich dynamic behavior with the formation and fusion of small clusters resembling molecules. The dynamics of this assembly is governed by an effective conservative energy that for large separations r decays as 1/r. Breaking the flow symmetry, these clusters can be made active.

Assembly and Speed in Ion-Exchange-Based Modular Phoretic Microswimmers

We report an experimental study on ion-exchange-based modular microswimmers in low-salt water. Cationic ion-exchange particles and passive cargo particles assemble into self-propelling complexes, showing self-propulsion at speeds of several micrometers per second over extended distances and times. We quantify the assembly and speed of the complexes for different combinations of ion-exchange particles and cargo particles, substrate types, salt types and concentrations, and cell geometries. Irrespective of the experimental boundary conditions, we observe a regular development of the assembly shape with increasing number of cargo. Moreover, the swimming speed increases stepwise upon increasing the number of cargo and then saturates at a maximum speed, indicating the active role of cargo in modular swimming. We propose a geometric model of self-assembly to describe the experimental observations in a qualitative way. Our study also provides some constraints for future theoretical modeling and simulation.

To make a glass—avoid the crystal

Colloidal model systems allow for a flexible tuning of particle sizes, particle spacings and mutual interactions at constant temperature. Colloidal suspensions typically crystallize as soon as the interactions get sufficiently strong and long-ranged. Several strategies have been successfully applied to avoid crystallization and instead produce colloidal glasses. Most of these amorphous solids are formed at high particle concentrations. This paper shortly reviews experimental attempts to produce amorphous colloidal solids using strategies based on topological, thermodynamic and kinetic considerations. We complement this overview by introducing a (transient) amorphous solid forming in a thoroughly deionized aqueous suspension of highly charged spheres at low salt concentration and very low volume fractions.

Large scale micro-photometry for high resolution pH-characterization during electro-osmotic pumping and modular micro-swimming

Micro-fluidic pumps as well as artificial micro-swimmers are conveniently realized exploiting phoretic solvent flows based on local gradients of temperature, electrolyte concentration or pH. We here present a facile micro-photometric method for monitoring pH gradients and demonstrate its performance and scope on different experimental situations including an electro-osmotic pump and modular micro-swimmers assembled from ion exchange resin beads and polystyrene colloids. In combination with the present microscope and DSLR camera our method offers a 2 \mu m spatial resolution at video frame rate over a field of view of 3920x2602 \mu m^2. Under optimal conditions we achieve a pH-resolution of 0.05 with about equal contributions from statistical and systematical uncertainties. Our quantitative micro-photometric characterization of pH gradients which develop in time and reach out several mm is anticipated to provide valuable input for reliable modeling and simulations of a large variety of complex flow situations involving pH-gradients including artificial micro-swimmers, microfluidic pumping or even electro-convection.

Modular approach to microswimming

The field of active matter in general and microswimming in particular has experienced a rapid and ongoing expansion over the last decade. A particular interesting aspect is provided by artificial autonomous microswimmers constructed from individual active and inactive functional components into self-propelling complexes. Such modular microswimmers may exhibit directed motion not seen for each individual component. In this review, we focus on the establishment and recent developments in the modular approach to microswimming. We introduce the bound and dynamic prototypes, show mechanisms and types of modular swimming and discuss approaches to control the direction and speed of modular microswimmers. We conclude by highlighting some challenges faced by researchers as well as promising directions for future research in the realm of modular swimming.

Colloidal electro-phoresis in the presence of symmetric and asymmetric electro-osmotic flow

We characterize the electro-phoretic motion of charged sphere suspensions in the presence of substantial electro-osmotic flow using a recently introduced small angle super-heterodyne dynamic light scattering instrument (ISASH-LDV). Operation in integral mode gives access to the particle velocity distribution over the complete cell cross-section. Obtained Doppler spectra are evaluated for electro-phoretic mobility, wall electro-osmotic mobility and particle diffusion coefficient. Simultaneous measurements of differing electro-osmotic mobilities leading to asymmetric solvent flow are demonstrated in a custom made electro-kinetic cell fitting standard microscopy slides as exchangeable sidewalls. The scope and range of our approach are discussed demonstrating the possibility of an internal calibration standard and using the simultaneously measured electro-kinetic mobilities in the interpretation of a microfluidic pumping experiment involving an inhomogeneous electric field and a complex solvent flow pattern.

Dynamics of Binary Active Clusters Driven by Ion-Exchange Particles

We present a framework to quantitatively predict the linear and rotational directed motion of synthetic modular microswimmers. To this end, we study binary dimers and characterize their approach motion as effective interactions within a minimal model. We apply this framework to the assembly of small aggregates composed of a cationic ion-exchange particle with up to five passive particles or anionic ion-exchange particles at dilute conditions. Particles sediment and move close to a substrate, above which the ion-exchange particles generate flow. This flow mediates long-range attractions leading to a slow collapse during which long-lived clusters of a few particles assemble. The effective interactions between unlike particles break Newtons third law. Depending on their symmetry, assemblies thus can become linear or circle swimmers, or remain inert (no directed motion).

Formation of a transient amorphous solid in low density aqueous charged sphere suspensions

Colloidal glasses formed from hard spheres, nearly hard spheres, ellipsoids and platelets or their attractive variants, have been studied in great detail. Complementing and constraining theoretical approaches and simulations, the many different types of model systems have significantly advanced our understanding of the glass transition in general. Despite their early prediction, however, no experimental charged sphere glasses have been found at low density, where the competing process of crystallization prevails. We here report the formation of a transient amorphous solid formed from charged polymer spheres suspended in thoroughly deionized water at volume fractions of 0.0002–0.01. From optical experiments, we observe the presence of short-range order and an enhanced shear rigidity as compared to the stable polycrystalline solid of body centred cubic structure. On a density dependent time scale of hours to days, the amorphous solid transforms into this stable structure. We further present preliminary dynamic light scattering data showing the evolution of a second slow relaxation process possibly pointing to a dynamic heterogeneity known from other colloidal glasses and gels. We compare our findings to the predicted phase behaviour of charged sphere suspensions and discuss possible mechanisms for the formation of this peculiar type of colloidal glass.