Aggregation-fragmentation and individual dynamics of active clusters.

A remarkable feature of active matter is the propensity to self-organize. One striking instance of this ability to generate spatial structures is the cluster phase, where clusters broadly distributed in size constantly move and evolve through particle exchange, breaking or merging. Here we propose an exhaustive description of the cluster dynamics in apolar active matter. Exploiting large statistics gathered on thousands of Janus colloids, we measure the aggregation and fragmentation rates and rationalize the resulting cluster size distribution and fluctuations. We also show that the motion of individual clusters is entirely consistent with a model positing random orientation of colloids. Our findings establish a simple, generic model of cluster phase, and pave the way for a thorough understanding of clustering in active matter.

Nanoscale Dynamics versus Surface Interactions: What Dictates Osmotic Transport?

The classical paradigm for osmotic transport has long related the induced-flow direction to the solute membrane interactions, with the low-to-high concentration flow a direct consequence of the solute rejection from the semipermeable membrane. In principle, the same was thought to occur for the newly demonstrated membrane-free osmotic transport named diffusio-osmosis. Using a recently proposed nanofluidic setup, we revisit this cornerstone of osmotic transport by studying the diffusio-osmotic flows generated at silica surfaces by either poly(ethylene)glycol polymers or ethanol molecules in aqueous solutions. Strikingly, both neutral solutes yield osmotic flows in the usual low to high concentration direction, in contradiction with their propensity to adsorb on silica. Considering theoretically and numerically the intricate nature of the osmotic response that combines molecular-scale surface interaction and near-wall dynamics, these findings are rationalized within a generalized framework. These elements constitute a step forward toward a finer understanding of osmotically driven flows, at the core of rapidly growing fields ranging from energy harvesting to active matter.

Chaotic mixing in effective compressible flows.

We study numerically joint mixing of salt and colloids by chaotic advection and how salt inhomogeneities accelerate or delay colloid mixing by inducing a velocity drift V(dp) between colloids and fluid particles as proposed in recent experiments [J. Deseigne et al., Soft Matter 10, 4795 (2014)]. We demonstrate that because the drift velocity is no longer divergence free, small variations to the total velocity field drastically affect the evolution of colloid variance σ(2) = 〈C(2)〉-〈C〉(2). A consequence is that mixing strongly depends on the mutual coherence between colloid and salt concentration fields, the short time evolution of scalar variance being governed by a new variance production term P = -〈C(2)∇ · V(dp)〉/2 when scalar gradients are not developed yet so that dissipation is weak. Depending on initial conditions, mixing is then delayed or enhanced, and it is possible to find examples for which the two regimes (fast mixing followed by slow mixing) are observed consecutively when the variance source term reverses its sign. This is indeed the case for localized patches modeled as Gaussian concentration profiles.

Osmotic flow through fully permeable nanochannels.

Osmosis across membranes is intrinsically associated with the concept of semipermeability. Here, however, we demonstrate that osmotic flow can be generated by solute gradients across nonselective, fully permeable nanochannels. Using a fluorescence imaging technique, we are able to measure the water flow rate inside single nanochannels to an unprecedented sensitivity of femtoliters per minute flow rates. Our results indicate the onset of a convective liquid motion under salinity gradients, from the higher to lower electrolyte concentration, which is attributed to diffusio-osmotic transport. To our knowledge, this is the first experimental evidence and quantitative investigation of this subtle interfacially driven transport, which need to be accounted for in nanoscale dynamics. Finally, diffusio-osmotic transport under a neutral polymer gradient is also demonstrated. The experiments highlight the entropic depletion of polymers that occurs at the nanochannel surface, resulting in convective flow in the opposite direction to that seen for electrolytes.

Dynamic clustering in active colloidal suspensions with chemical signaling.

In this Letter, we explore experimentally the phase behavior of a dense active suspension of self-propelled colloids. In addition to a solidlike and gaslike phase observed for high and low densities, a novel cluster phase is reported at intermediate densities. This takes the form of a stationary assembly of dense aggregates-resulting from a permanent dynamical merging and separation of active colloids-whose average size grows with activity as a linear function of the self-propelling velocity. While different possible scenarios can be considered to account for these observations-such as a generic velocity weakening instability recently put forward-we show that the experimental results are reproduced mathematically by a chemotactic aggregation mechanism, originally introduced to account for bacterial aggregation and accounting here for diffusiophoretic chemical interaction between colloidal swimmers.

Boosting migration of large particles by solute contrasts.

Brownian diffusion is a keystone concept in a large variety of domains, from physics, chemistry to biology. Diffusive transport controls situations as diverse as reaction-diffusion processes in biology and chemistry, Brownian ratchet processes, dispersion in microfluidic devices or even double-diffusive instability and salt-fingering phenomena in the context of ocean mixing. Although these examples span a broad range of length scales, diffusive transport becomes increasingly inefficient for larger particles. Applications, for example, in microfluidics, usually have recourse to alternative driving methods involving external sources to induce and control migration. Here, we demonstrate experimentally a strongly enhanced migration of large particles, achieved by slaving their dynamics to that of a fast carrier species, a dilute salt. The underlying fast salt diffusion leads to an apparent diffusive-like dynamics of the large particles, which is up to two orders of magnitude faster than their natural 'bare' diffusion. Moreover both spreading and focusing of the particle assembly can be achieved on demand. A model description shows a remarkable quantitative agreement with all measured data. Applications of this process are illustrated in microfluidics for filtering and concentrating operations, as well as in conjunction with standard hydrodynamic focusing. In a wider perspective, this mechanism can affect a broad range of scales and phenomena, from biological transport to the dispersion of sediments and pollutants in oceanographic situations.

Nanoscale flow on a bubble mattress: effect of surface elasticity.

We present an experimental study of the elastic properties of a superhydrophobic surface in the Cassie regime, due to the gas bubbles trapped at the liquid-solid interface. We use a surface force apparatus to measure the force response to an oscillating drainage flow between a sphere and the surface. We show that the force response allows to determine the surface elasticity without contact, using the liquid film as a probe. The elasticity of the bubble mattress is dominated by the meniscii stiffness, and its determination enables us to probe the shape of these meniscii. Another effect of surface elasticity is to decrease the viscous friction. We show that this effect can be wrongly attributed to rate dependant boundary slippage if elastohydrodynamics is not taken into account.

Using surface force apparatus, diffusion and velocimetry to measure slip lengths.

Determining the slip lengths for liquids flowing close to smooth walls is challenging. The reason lies in the fact that the scales that must be addressed range between a few and hundreds of nanometres. Several techniques have been used over the last few years. Here, we consider three of them based on surface force apparatus, diffusion and velocimetry, respectively. The descriptions offered here incorporate recent instrumental progress made in the field.

Slippage of water past superhydrophobic carbon nanotube forests in microchannels.

We present in this Letter an experimental characterization of liquid flow slippage over superhydrophobic surfaces made of carbon nanotube forests, incorporated in microchannels. We make use of a particle image velocimetry technique to achieve the submicrometric resolution on the flow profile necessary for accurate measurement of the surface hydrodynamic properties. We demonstrate boundary slippage on the Cassie superhydrophobic state, associated with slip lengths of a few microns, while a vanishing slip length is found in the Wenzel state when the liquid impregnates the surface. Varying the lateral roughness scale L of our carbon nanotube forest-based superhydrophobic surfaces, we demonstrate that the slip length varies linearly with L in line with theoretical predictions for slippage on patterned surfaces.

Boundary slip on smooth hydrophobic surfaces: intrinsic effects and possible artifacts.

We report an accurate determination of the hydrodynamic boundary condition of simple liquids flowing on smooth hydrophobic surfaces using a dynamic surface force apparatus equipped with two independent subnanometer resolution sensors. The boundary slip observed is well defined and does not depend on the scale of investigation from one to several hundreds of nanometers, nor on shear rate up to 5 x 10(3)s(-1). The slip length of 20 nm is in good agreement with theory and numerical simulations concerning smooth nonwetting surfaces. These results disagree with previous data in the literature reporting very high boundary slip on similar systems. We discuss possible origins of large slip length on smooth hydrophobic surfaces due to their contamination by hydrophobic particles.

Dynamics of simple liquids at heterogeneous surfaces: molecular-dynamics simulations and hydrodynamic description.

In this paper we consider the effect of surface heterogeneity on the slippage of fluid, using two complementary approaches. First, MD simulations of a corrugated hydrophobic surface have been performed. A dewetting transition, leading to a super-hydrophobic state, is observed for pressure below a "capillary" pressure. Conversely, a very large slippage of the fluid on this composite interface is found in this super-hydrophobic state. Second, we propose a macroscopic estimate of the effective slip length on the basis of continuum hydrodynamics, in order to rationalize the previous MD results. This calculation allows to estimate the effect of a heterogeneous slip length pattern at the composite interface. Comparison between the two approaches shows that they are in good agreement at low pressure, but highlights the role of the exact shape of the liquid-vapor interface at higher pressure. These results confirm that small variations in the roughness of a surface can lead to huge differences in the slip effect. On the basis of these results, we propose some guidelines to design highly slippery surfaces, motivated by potential applications in microfluidics.

Adhesion between weakly rough beads.

Cohesion effects are of prime importance in powders and granular media, and they are strongly affected by the roughness of the grain surface. We report measurements of the adhesion force between surfaces of Pyrex having a nanometric roughness, with a surface force apparatus. The two surfaces are immersed in liquid n-dodecane. The adhesion force measured is much smaller than expected in the case of smooth surfaces. We find that the adhesion force depends on the maximal load that has been applied on the surfaces, but does not depend on the time during which they have been in contact. We propose a model of plastic deformation of the small asperities in a macroscopic Hertz contact which is in good agreement with the experimental data.

Nanorheology: An investigation of the boundary condition at hydrophobic and hydrophilic interfaces.

It has been shown that the flow of a simple liquid over a solid surface can violate the so-called no-slip boundary condition. We investigate the flow of polar liquids, water and glycerol, on a hydrophilic Pyrex surface and a hydrophobic surface made of a Self-Assembled Monolayer of OTS (octadecyltrichlorosilane) on Pyrex. We use a Dynamic Surface Force Apparatus (DSFA) which allows one to study the flow of a liquid film confined between two surfaces with a nanometer resolution. No-slip boundary conditions are found for both fluids on hydrophilic surfaces only. Significant slip is found on the hydrophobic surfaces, with a typical length of one hundred nanometers.