Emulsions in microfluidic channels with asymmetric boundary conditions and directional surface roughness: stress and rheology.

The flow of emulsions in confined microfluidic channels is affected by surface roughness. Directional roughness effects have recently been reported in channels with asymmetric boundary conditions featuring a flat wall, and a wall textured with directional roughness, the latter promoting a change in the velocity profiles when the flow direction of emulsions is inverted [D. Filippi et al., Adv. Mater. Technol., 2023, 8, 2201748]. An operative protocol is needed to reconstruct the stress profile inside the channel from velocity data to shed light on the trigger of the directional response. To this aim, we performed lattice Boltzmann numerical simulations of the flow of model emulsions with a minimalist model of directional roughness in two dimensions: a confined microfluidic channel with one flat wall and the other patterned by right-angle triangular-shaped posts. Simulations are essential to develop a protocol based on mechanical arguments to reconstruct stress profiles. Hence, one can analyze data to relate directional effects in velocity profiles to different rheological responses close to the rough walls associated with opposite flow directions. We finally show the universality of this protocol by applying it to other realizations of directional roughness by considering experimental data on emulsions in a microfluidic channel featuring a flat wall and a wall textured by herringbone-shaped roughness.

Resonance Modes of Water Drops Pinned to a Vibrating Rectangular Post.

We studied the effects of vertical vibrations on a water drop that was pinned to the sharp edges of a rectangular post. By varying the frequency and amplitude of the vertical displacement, distinct resonance peaks were observed using a simple optical technique. The vibrational spectra of the first two modes exhibited two closely spaced peaks, which corresponded to standing waves that exist along the major and minor contour lengths of the drops. The values of the resonance frequencies can be explained rather well by a simple model, which was originally proposed for axially symmetric drops.

Trifurcated Splitting of Water Droplets on Engineered Lithium Niobate Surfaces.

Controlled splitting of liquid droplets is a key function in many microfluidic applications. In recent years, various methodologies have been used to accomplish this task. Here, we present an optofluidic technique based on an engineered surface formed by coating a z-cut iron-doped lithium niobate crystal with a lubricant-infused layer, which provides a very slippery surface. Illuminating the crystal with a light spot induces surface charges of opposite signs on the two crystal faces because of the photovoltaic effect. If the light spot is sufficiently intense, millimetric water droplets placed near the illuminated spot split into two charged fragments, one fragment being trapped by the bright spot and the other moving away from it. The latter fragment does not move randomly but rather follows one of three well-defined trajectories separated by 120°, which reflect the anisotropic crystalline structure of Fe:LiNbO3. Numerical simulations explain the behavior of water droplets in the framework of the forces induced by the interplay of pyroelectric, piezoelectric, and photovoltaic effects, which originate simultaneously inside the illuminated crystal. Such a synergetic effect can provide a valuable feature in applications that require splitting and coalescence of droplets, such as chemical microreactors and biological encapsulation and screening.

Shaking Device for Homogeneous Dispersion of Magnetic Beads in Droplet Microfluidics.

Magnetic beads (or particles) having a size between 1 and 5 µm are largely used in many biochemical assays devoted to both purification and quantification of cells, nucleic acids, or proteins. Unfortunately, the use of these beads within microfluidic devices suffers from natural precipitation because of their size and density. The strategies applied thus far to cells or polymeric particles cannot be extended to magnetic beads, mainly due to their magnetization and their higher densities. We report an effective shaking device capable of preventing the sedimentation of beads that are stored in a custom PCR tube. After the characterization of the operating principle, the device is validated for magnetic beads in droplets, leading to an equal distribution between the droplets, barely affecting their generation.

Sliding and rolling of yield stress fluid droplets on highly slippery lubricated surfaces.

HYPOTHESIS: Droplets of yield stress fluids (YSFs), i.e. fluids that can flow only if they are subjected to a stress above a critical value and otherwise deform like solids, hardly move on solid surfaces due to their high viscosity. The use of highly slippery lubricated surfaces can shed light on the mobility of YSF droplets, which include everyday soft materials, such as toothpaste or mayonnaise, and biological fluids, such as mucus. EXPERIMENTS: The spreading and mobility of droplets of aqueous solutions of swollen Carbopol microgels were studied on lubricant infused surfaces. These solutions represent a model system of YSFs. Dynamical phase diagrams were established by varying the concentration of the solutions and the inclination angle of the surfaces. FINDINGS: Carbopol droplets deposited on lubricated surfaces could move even at low inclination angles. The droplets were found to slide because of the slip of the flowing oil that covered the solid substrate. However, as the descending speed increased, the droplets rolled down. Rolling was favored at high inclinations and low concentrations. A simple criterion based on the ratio between the yield stress of the Carbopol suspensions and the gravitational stress acting on the Carbopol droplets was found to nicely identify the transition between the two regimes.

Determination of the Dielectrophoretic Force Induced by the Photovoltaic Effect on Lithium Niobate.

The actuation of droplets on a surface is extremely relevant for microfluidic applications. In recent years, various methodologies have been used. A promising solution relies on iron-doped lithium niobate crystals that, when illuminated, generate an evanescent electric field in the surrounding space due to the photovoltaic effect. This field can be successfully exploited to control the motion of water droplets. Here, we present an experimental method to determine the attractive force exerted by the evanescent field. It consists of the analysis of the elongation of a pendant droplet and its detachment from the suspending syringe needle, caused by the illumination of an iron-doped lithium niobate crystal. We show that this interaction resembles that obtained by applying a voltage between the needle and a metallic substrate, and a quantitative investigation of these two types of actuation yields similar results. Pendant droplet tensiometry is then demonstrated to offer a simple solution for quickly mapping out the force at different distances from the crystal, generated by the photovoltaic effect and its temporal evolution, providing important quantitative data for the design and characterization of optofluidic devices based on lithium niobate crystals.

Microfluidic Strategies for Extracellular Vesicle Isolation: Towards Clinical Applications.

Extracellular vesicles (EVs) are double-layered lipid membrane vesicles released by cells. Currently, EVs are attracting a lot of attention in the biological and medical fields due to their role as natural carriers of proteins, lipids, and nucleic acids. Thus, they can transport useful genomic information from their parental cell through body fluids, promoting cell-to-cell communication even between different organs. Due to their functionality as cargo carriers and their protein expression, they can play an important role as possible diagnostic and prognostic biomarkers in various types of diseases, e.g., cancers, neurodegenerative, and autoimmune diseases. Today, given the invaluable importance of EVs, there are some pivotal challenges to overcome in terms of their isolation. Conventional methods have some limitations: they are influenced by the starting sample, might present low throughput and low purity, and sometimes a lack of reproducibility, being operator dependent. During the past few years, several microfluidic approaches have been proposed to address these issues. In this review, we summarize the most important microfluidic-based devices for EV isolation, highlighting their advantages and disadvantages compared to existing technology, as well as the current state of the art from the perspective of the use of these devices in clinical applications.

Morphological Transitions of Water Channels Induced by Vertical Vibrations.

We report the results of comprehensive experiments and numerical calculations of interfacial morphologies of water confined to the hydrophilic top face of rectangular posts subjected to vertical vibrations. In response to mechanical driving, an initially flat liquid channel is collected into a liquid bulge that forms in the center of the rectangular post if the acceleration exceeds a certain threshold. The bulge morphology persists after the driving is switched off, in agreement with the morphological bistability of static interfacial shapes on posts with large length-to-width ratios. In a narrow frequency band, the channel does not decay into a bulge at any acceleration amplitude, but displays irregular capillary waves and sloshing instead. On short posts, however, a liquid bulge can be dynamically sustained through vertical vibrations but quickly decays into a homogeneous channel after the external driving is stopped. To explain the dynamic bulging of the liquid interface, we propose an effective lifting force pulling on the drop's slowly moving center of mass in the presence of fast oscillation modes.

Division of Ferrofluid Drops Induced by a Magnetic Field.

We report a comprehensive study of the division of ferrofluid drops caused by their interaction with a permanent magnet. As the magnet gradually approaches the sessile drop, the drop deforms into a spiked cone and then divides into two daughter droplets. This process is the result of a complex interplay between the polarizing effect caused by the magnetic field and the magnetic attraction due to the field gradient. As a first attempt to describe it, during each scan we identify two characteristic distances between the magnet and the drop: zmax, corresponding to the drop reaching its maximum height, and zsaddle, corresponding to the formation of a saddle point on the drop peak identifying the beginning of the drop breakup. We have investigated the location of these two points using sessile drops of ferrofluid water solutions at various concentrations and volumes, deposited on four surfaces of different wettability. An empirical scaling law based on dimensionless variables is found to accurately describe these experimental observations. We have also measured the maximum diameter of the drops right before the division and found that it is very close to a critical size, which depends on the magnetic attraction.

Wall accumulation of bacteria with different motility patterns.

We systematically investigate the role of different swimming patterns on the concentration distribution of bacterial suspensions confined between two flat walls, by considering wild-type motility Escherichia coli and Pseudomonas aeruginosa, which perform Run and Tumble and Run and Reverse patterns, respectively. The experiments count motile bacteria at different distances from the bottom wall. In agreement with previous studies, an accumulation of motile bacteria close to the walls is observed. Different wall separations, ranging from 100 to 250µm, are tested. The concentration profiles result to be independent on the motility pattern and on the walls' separation. These results are confirmed by numerical simulations, based on a collection of self-propelled dumbbells-like particles interacting only through steric interactions. The good agreement with the simulations suggests that the behavior of the investigated bacterial suspensions is determined mainly by steric collisions and self-propulsion, as well as hydrodynamic interactions.

Wall fluidization in two acts: from stiff to soft roughness.

Fluidization of soft glassy materials (SGMs) in microfluidic channels is affected by the wall roughness in the form of microtexturing. When SGMs flow across microgrooves, their constituents are likely trapped within the grooves' gap, and the way they are released locally modifies the fluidization close to the walls. By leveraging a suitable combination of experiments and numerical simulations on concentrated emulsions (a model SGM), we quantitatively report the existence of two physically different scenarios. When the gap is large compared to the droplets in the emulsion, the droplets hit the solid obstacles and easily escape scrambling with their neighbors. Conversely, as the gap spacing is reduced, droplets get trapped inside, creating a "soft roughness" layer, i.e. a complementary series of deformable posts from which overlying droplets are in turn released. In both cases, the induced fluidization scales with the grooves' density, although with a reduced prefactor for narrow gaps, accounting for the softness of the roughness. Both scenarios are also well distinguished via the statistics of the droplets displacement field close to the walls, with large deviations induced by the surface roughness, depending on its stiffness.

Fluidization and wall slip of soft glassy materials by controlled surface roughness.

We present a comprehensive study of concentrated emulsions flowing in microfluidic channels, one wall of which is patterned with micron-size equally spaced grooves oriented perpendicularly to the flow direction. We find a scaling law describing the roughness-induced fluidization as a function of the density of the grooves, thus fluidization can be predicted and quantitatively regulated. This suggests common scenarios for droplet trapping and release, potentially applicable for other jammed systems as well. Numerical simulations confirm these views and provide a direct link between fluidization and the spatial distribution of plastic rearrangements.

Stretching of viscoelastic drops in steady sliding.

The sliding of non-Newtonian drops down planar surfaces results in a complex, entangled balance between interfacial forces and non-linear viscous dissipation, which has been scarcely inspected. In particular, a detailed understanding of the role played by the polymer flexibility and the resulting elasticity of the polymer solution is still lacking. To this aim, we have considered polyacrylamide (PAA) solutions of different molecular weights, suspended either in water or in glycerol/water mixtures. In contrast to drops of stiff polymers, drops of flexible polymers exhibit a remarkable elongation in steady sliding. This difference is most likely attributed to variation of viscous bending as a consequence of variation of shear thinning. Moreover, an "optimal elasticity" of the polymer seems to be required for this drop elongation to be visible. We have complemented experimental results with numerical simulations of a viscoelastic FENE-P drop. This has been a decisive step to unraveling how a change of the elastic parameters (e.g. polymer relaxation time, maximum extensibility) affects the dimensionless sliding velocity.

Deviation of sliding drops at a chemical step.

The motion of partially wetting liquid drops in contact with a solid surface is strongly affected by contact angle hysteresis and interfacial pinning. However, the majority of models proposed for drops sliding over chemical surface patterns consistently neglect the difference between advancing and receding contact angles. In this article, we present a joint experimental and numerical study of the interaction of gravity-driven drops with a chemical step formed at the junction between a hydrophilic and a hydrophobic region. It demonstrates the strong impact of a contact angle hysteresis contrast on the motion of drops at a linear chemical step. Surprisingly, the smallest driving force required to drag the drop across the step onto the lower hydrophobic surface is not observed at a right angle of incidence. Our model reveals that the non-monotonous response of this passive drop 'filter' is solely due to the higher advancing contact angle on the lower surface, and creates an instance where drop motion is affected by dissipation at the contact line rather than by surface energy.

Static Magnetowetting of Ferrofluid Drops.

We report results of a comprehensive study of the wetting properties of sessile drops of ferrofluid water solutions at various concentrations deposited on flat substrates and subjected to the action of permanent magnets of different sizes and strengths. The amplitude and the gradient of the magnetic field experienced by the ferrofluid are changed by varying the magnets and their distance to the surface. Magnetic forces up to 100 times the gravitational one and magnetic gradients up to 1 T/cm are achieved. A rich phenomenology is observed, ranging from flattened drops caused by the magnetic attraction to drops extended normally to the substrate because of the normal traction of the magnetic field. We find that the former effect can be conveniently described in terms of an effective Bond number that compares the effective drop attraction with the capillary force, whereas the drop's vertical elongation is effectively expressed by a dimensionless number S, which compares the pressure jump at the ferrofluid interface because of the magnetization with the capillary pressure.

Single-File Escape of Colloidal Particles from Microfluidic Channels.

Single-file diffusion is a ubiquitous physical process exploited by living and synthetic systems to exchange molecules with their environment. It is paramount to quantify the escape time needed for single files of particles to exit from constraining synthetic channels and biological pores. This quantity depends on complex cooperative effects, whose predominance can only be established through a strict comparison between theory and experiments. By using colloidal particles, optical manipulation, microfluidics, digital microscopy, and theoretical analysis we uncover the self-similar character of the escape process and provide closed-formula evaluations of the escape time. We find that the escape time scales inversely with the diffusion coefficient of the last particle to leave the channel. Importantly, we find that at the investigated microscale, bias forces as tiny as 10^{-15} N determine the magnitude of the escape time by drastically reducing interparticle collisions. Our findings provide crucial guidelines to optimize the design of micro- and nanodevices for a variety of applications including drug delivery, particle filtering, and transport in geometrical constrictions.

Sliding droplets of Xanthan solutions: A joint experimental and numerical study.

We have investigated the sliding of droplets made of solutions of Xanthan, a stiff rodlike polysaccharide exhibiting a non-Newtonian behavior, notably characterized by a shear thinning viscosity accompanied by the emergence of normal stress difference as the polymer concentration is increased. These experimental results are quantitatively compared with those of Newtonian fluids (water). The impact of the non-Newtonian behavior on the sliding process was shown through the relation between the average dimensionless velocity (i.e. the capillary number) and the dimensionless volume forces (i.e. the Bond number). To this aim, it is needed to define operative strategies to compute the capillary number for the shear thinning fluids and compare with the corresponding Newtonian case. The resulting capillary number for the Xanthan solutions scales linearly with the Bond number at small inclinations, as well known for Newtonian fluids, while it shows a plateau as the Bond number is increased. Experimental data were complemented with lattice Boltzmann numerical simulations of sliding droplets, aimed to disentangle the specific contribution of shear thinning and elastic effects on the sliding behavior. In particular the deviation from the linear (Newtonian) trend is more likely attributed to the emergence of normal stresses inside the non-Newtonian droplet.

Frictional transition from superlubric islands to pinned monolayers.

The inertial sliding of physisorbed submonolayer islands on crystal surfaces contains unexpected information on the exceptionally smooth sliding state associated with incommensurate superlubricity and on the mechanisms of its disappearance. Here, in a joint quartz crystal microbalance and molecular dynamics simulation case study of Xe on Cu(111), we show how superlubricity emerges in the large size limit of naturally incommensurate Xe islands. As coverage approaches a full monolayer, theory also predicts an abrupt adhesion-driven two-dimensional density compression on the order of several per cent, implying a hysteretic jump from superlubric free islands to a pressurized commensurate immobile monolayer. This scenario is fully supported by the quartz crystal microbalance data, which show remarkably large slip times with increasing submonolayer coverage, signalling superlubricity, followed by a dramatic drop to zero for the dense commensurate monolayer. Careful analysis of this variety of island sliding phenomena will be essential in future applications of friction at crystal/adsorbate interfaces.

Active Brownian particles escaping a channel in single file.

Active particles may happen to be confined in channels so narrow that they cannot overtake each other (single-file conditions). This interesting situation reveals nontrivial physical features as a consequence of the strong interparticle correlations developed in collective rearrangements. We consider a minimal two-dimensional model for active Brownian particles with the aim of studying the modifications introduced by activity with respect to the classical (passive) single-file picture. Depending on whether their motion is dominated by translational or rotational diffusion, we find that active Brownian particles in single file may arrange into clusters that are continuously merging and splitting (active clusters) or merely reproduce passive-motion paradigms, respectively. We show that activity conveys to self-propelled particles a strategic advantage for trespassing narrow channels against external biases (e.g., the gravitational field).

Thermolubricity of gas monolayers on graphene.

Nanofriction of Xe, Kr and N2 monolayers deposited on graphene was explored with a quartz crystal microbalance (QCM) at temperatures between 25 and 50 K. Graphene was grown by chemical vapour deposition and transferred to the QCM electrodes with a polymer stamp. It was found to strongly adhere to the gold electrodes at temperatures as low as 5 K and at frequencies up to 5 MHz. At low temperatures, the Xe monolayers are fully pinned to the graphene surface. Above 30 K, the Xe film slides and the depinning onset coverage beyond which the film starts sliding decreases with temperature. Similar measurements repeated on bare gold show an enhanced slippage of the Xe films and a decrease of the depinning temperature below 25 K. Nanofriction measurements of Kr and N2 confirm this scenario. This thermolubric behaviour is explained in terms of a recent theory of the size dependence of static friction between adsorbed islands and crystalline substrates.