Transitioning to confined spaces impacts bacterial swimming and escape response.

Symbiotic bacteria often navigate complex environments before colonizing privileged sites in their host organism. Chemical gradients are known to facilitate directional taxis of these bacteria, guiding them toward their eventual destination. However, less is known about the role of physical features in shaping the path the bacteria take and defining how they traverse a given space. The flagellated marine bacterium Vibrio fischeri, which forms a binary symbiosis with the Hawaiian bobtail squid, Euprymna scolopes, must navigate tight physical confinement during colonization, squeezing through a tissue bottleneck constricting to ∼2 µm in width on the way to its eventual home. Using microfluidic in vitro experiments, we discovered that V. fischeri cells alter their behavior upon entry into confined space, straightening their swimming paths and promoting escape from confinement. Using a computational model, we attributed this escape response to two factors: reduced directional fluctuation and a refractory period between reversals. Additional experiments in asymmetric capillary tubes confirmed that V. fischeri quickly escape from confined ends, even when drawn into the ends by chemoattraction. This avoidance was apparent down to a limit of confinement approaching the diameter of the cell itself, resulting in a balance between chemoattraction and evasion of physical confinement. Our findings demonstrate that nontrivial distributions of swimming bacteria can emerge from simple physical gradients in the level of confinement. Tight spaces may serve as an additional, crucial cue for bacteria while they navigate complex environments to enter specific habitats.

Confinement-Dependent Diffusiophoretic Transport of Nanoparticles in Collagen Hydrogels.

The transport of nanoparticles in biological hydrogels is often hindered by the strong confinement of the media, thus limiting important applications such as drug delivery and disinfection. Here, we investigate nanoparticle transport in collagen hydrogels driven by diffusiophoresis. Contrary to common expectations for boundary confinement effects where the confinement hinders diffusiophoresis, we observe a nonmonotonic behavior in which maximum diffusiophoretic mobility is observed at intermediate confinement. We find that such behavior is a consequence of the interplay between multiple size-dependent effects. Our results display the utility of diffusiophoresis for enhanced nanoparticle transport in physiologically relevant conditions under tight confinement, suggesting a potential strategy for drug delivery in compressed tissues.

Formation of a colloidal band via pH-dependent electrokinetics.

Electroosmosis on nonuniformly charged surfaces often gives rise to intriguing flow behaviors, which can be utilized in applications such as mixing processes and designing micromotors. Here, we demonstrate nonuniform electroosmosis induced by electrochemical reactions. Water electrolysis creates pH gradients near the electrodes that cause a spatiotemporal change in the wall zeta potential, leading to nonuniform electroosmosis. Such nonuniform EOFs induce multiple vortices, which promote the continuous accumulation of particles that subsequently form a colloidal band. The band develops vertically into a "wall" of particles that spans from the bottom to the top surface of the chamber. Such a flow-driven colloidal band can be potentially used in colloidal self-assembly and separation processes irrespective of the particle surface properties. For instance, we demonstrate these vortices can promote rapid segregation of soft colloids such as oil droplets and fat globules.

Self-Formation of Superhydrophobic Surfaces through Interfacial Energy Engineering between Liquids and Particles.

The superhydrophobic surface has been used in ultradry surface applications, such as the maritime industry, windshields, non-sticky surfaces, anti-icing surfaces, self-cleaning surfaces, and so forth. However, one of the main hurdles for the production of superhydrophobic surfaces is high-cost fabrication methods. Here, we report a handy process of self-synthesis fabrication of superhydrophobic surfaces with daily supplies. Driven by the physics of biscuit dunking, we introduce a method to self-synthesize superhydrophobic surfaces from daily supplies by coating a substrate with a liquid (liquids of paraffin from candles or polydimethylsiloxane) and subsequently sprinkling powders (food-desiccant silica, alumina, sugar, salt, or flour). A mechanistic study revealed that the capillary force, governed by surface energy difference, liquid viscosity, and powder pore size, draws the liquid solution into the porous channels within the powders. The entire surface of powders, in turn, is covered with the low-surface-energy liquid to maintain the porosity, creating a 3D porous nanostructure, resulting in a water contact angle over 160°. This work provides a scientific understanding that technological developments are closely related to the science that can be seen in our daily lives. Also, we believe that further intensive studies extended from this work could enable to home-fabricate a superhydrophobic surface, such as a bathtub and sink in bathrooms and a cooking area and sink in kitchens.

Colloid Separation by CO2-Induced Diffusiophoresis.

We present a microfluidic crossflow separation of colloids enabled by the dissolution of CO2 gas in aqueous suspensions. The dissolved CO2 dissociates into H+ and HCO3- ions, which are efficient candidates for electrolytic diffusiophoresis, because of the fast diffusion of protons. By exposing CO2 gas to one side of a microfluidic flow channel, a crossflow gradient can be created, enabling the crossflow diffusiophoresis of suspended particles. We develop a simple two-dimensional model to describe the coupled transport dynamics that is due to the competition of advection and diffusiophoresis. Furthermore, we show that oil nanoemulsions can be effectively separated by utilizing highly charged particles as a carrier vehicle, which is otherwise difficult to achieve. These results demonstrate a portable, versatile method for separating particles in broad applications including oil extraction, drug delivery, and bioseparation.

Light-triggered explosion of lipid vesicles.

Lipid vesicles have received considerable interest because of their applications to in vitro reductionist cell membrane models as well as therapeutic delivery vehicles. In these contexts, the mechanical response of vesicles in nonequilibrium environments plays a key role in determining the corresponding dynamics. A common understanding of the response of lipid vesicles upon exposure to a hypotonic solution is a characteristic pulsatile behavior. Recent experiments, however, have shown vesicles exploding under an osmotic shock generated by photo-reactions, yet the explanatory mechanism is unknown. Here we present a generalized biophysical model incorporating a stochastic account of membrane rupture to describe both swell-burst-reseal cycling and exploding dynamics. This model agrees well with experimental observations, and it unravels that the sudden osmotic shock strains the vesicle at an extreme rate, driving the vesicle into buckling instabilities responsible for membrane fragmentation, i.e. explosion. Our work not only advances the fundamental framework for non-equilibrium vesicle dynamics under osmotic stress, but also offers design guidelines for programmable vesicle-encapsulated substance release in therapeutic carriers.

Correction: Light-triggered explosion of lipid vesicles.

Correction for 'Light-triggered explosion of lipid vesicles' by Vinit Kumar Malik et al., Soft Matter, 2020, DOI: 10.1039/d0sm01027h.

Characterization of surface-solute interactions by diffusioosmosis.

The accurate measurement of wall zeta potentials and solute-surface interaction length scales for electrolyte and non-electrolyte solutes, respectively, is critical to the design of many biomedical and microfluidic applications. We present a novel microfluidic approach using diffusioosmosis for measuring either the zeta potentials or the characteristic interaction length scales for surfaces exposed to, respectively, electrolyte or non-electrolyte solutes. When flows containing different solute concentrations merge in a junction, local solute concentration gradients can drive diffusioosmotic flow due to electrokinetic, steric, and other interactions between the solute molecules and solid surfaces. We demonstrate a microfluidic system consisting of a long, narrow pore connecting two large side channels in which solute concentration gradients drive diffusioosmosis within the pore, resulting in predictable fluid velocity/pressure and solute profiles. Furthermore, we present analytical results and a methodology to determine the zeta potential or interaction length scale for the pore surfaces based on the solute concentrations in the main side channels, the flow rate in the pore, and the pressure drop across the pore. We apply this method to the experimental data of Lee et al. to predict the zeta potentials of their system, and we use 3D numerical simulations to validate the theory and show that end effects caused by the junctions are negligible for a wide range of parameters. Because the dynamics in the proposed system are driven by diffusioosmosis, this technique does not suffer from certain disadvantages associated with the use of sensitive electronics in traditional zeta potential measurement approaches such as streaming potential, streaming current, or electroosmosis. To the best of our knowledge this is the first flow-based approach to characterize surface/solute interactions with non-electrolyte solutes.

Diffusiophoresis in ionic surfactants: effect of micelle formation.

We explore the consequences of micelle formation for diffusiophoresis of charged colloidal particles in ionic surfactant concentration gradients, using a quasi-chemical association model for surfactant self assembly. The electrophoretic contribution to diffusiophoresis is determined by re-arranging the Nernst-Planck equations, and the chemiphoretic contribution is estimated by making plausible approximations for the density profiles in the electrical double layer surrounding the particle. For sub-micellar solutions we find that a particle will typically be propelled down the concentration gradient, although electrophoresis and chemiphoresis are finely balanced and the effect is sensitive to the detailed parameter choices and simplifying assumptions in the model. Above the critical micelle concentration (CMC), diffusiophoresis becomes much weaker and may even reverse sign, due to the fact that added surfactant goes into building micelles and not augmenting the monomer or counterion concentrations. We present detailed calculations for sodium dodecyl sulfate (SDS), finding that the typical drift speed for a colloidal particle in a ∼100 µm length scale SDS gradient is ∼1 µm s-1 below the CMC, falling to ⪅0.2 µm s-1 above the CMC. These predictions are broadly in agreement with recent experimental work.

Particle entrainment in dead-end pores by diffusiophoresis.

The transport of particulate matter to and from dead-end pores is difficult to achieve due to confinement effects. Diffusiophoresis is a phenomenon that results in the controlled motion of colloids along solute concentration gradients. Thus, by establishing an electrolyte concentration gradient within dead-end pores, it is possible to induce the flow of particles into and out of the pores via diffusiophoresis, as has been demonstrated recently. In this paper, we explain the pore-scale mechanism by which individual colloids are entrained in dead-end pores by diffusiophoresis. We flow particles past a series of dead-end pores in the presence of a solute concentration gradient. Our results reveal that particles execute pore-to-pore hops before ultimately being captured. We categorize an event as particle capture when the particle's trajectory terminates within the dead-end pore. Experiments and numerical simulations demonstrate that particle capture only occurs when flowing particles are positioned sufficiently close to the pore entry. Outside this capture region, the particles have insufficient diffusiophoretic velocities to induce capture and their dynamics are largely dominated by their free-stream advective velocities. We observe that the particles move closer to the device wall as they hop, thereby reducing the effect of flow advection and increasing that of diffusiophoresis. These results enhance our understanding of suspension dynamics in a driven system and have implications for the development, design, and optimization of diffusiophoretic platforms for drug delivery, cosmetics, and material recovery.

Size-dependent control of colloid transport via solute gradients in dead-end channels.

Transport of colloids in dead-end channels is involved in widespread applications including drug delivery and underground oil and gas recovery. In such geometries, Brownian motion may be considered as the sole mechanism that enables transport of colloidal particles into or out of the channels, but it is, unfortunately, an extremely inefficient transport mechanism for microscale particles. Here, we explore the possibility of diffusiophoresis as a means to control the colloid transport in dead-end channels by introducing a solute gradient. We demonstrate that the transport of colloidal particles into the dead-end channels can be either enhanced or completely prevented via diffusiophoresis. In addition, we show that size-dependent diffusiophoretic transport of particles can be achieved by considering a finite Debye layer thickness effect, which is commonly ignored. A combination of diffusiophoresis and Brownian motion leads to a strong size-dependent focusing effect such that the larger particles tend to concentrate more and reside deeper in the channel. Our findings have implications for all manners of controlled release processes, especially for site-specific delivery systems where localized targeting of particles with minimal dispersion to the nontarget area is essential.

Enhanced Boiling Heat Transfer using Self-Actuated Nanobimorphs.

We present a new concept of a structured surface for enhanced boiling heat transfer that is capable of self-adapting to the local thermal conditions. An array of freestanding nanoscale bimorphs, a structure that consists of two adjoining materials with a large thermal expansion mismatch, is able to deform under local temperature change. Such a surface gradually deforms as the nucleate boiling progresses due to the increase in the wall superheat. The deformation caused by the heated surface is shown to be favorable for boiling heat transfer, leading to about 10% of increase in the critical heat flux compared to a regular nanowire surface. A recently developed theoretical model that accounts for the critical instability wavelength of the vapor film and the capillary wicking force successfully describes the critical heat flux enhancement for the nanobimorph surface with a good quantitative agreement.

Diffusiophoresis in one-dimensional solute gradients.

The diffusiophoretic motion of suspended colloidal particles under one-dimensional solute gradients is solved using numerical and analytical techniques. Similarity solutions are developed for the injection and withdrawal dynamics of particles into semi-infinite pores. Furthermore, a method of characteristics formulation of the diffusion-free particle transport model is presented and integrated to realize particle trajectories. Analytical solutions are presented for the limit of small particle diffusiophoretic mobility Γp relative to the solute diffusivity Ds for particle motions in both semi-infinite and finite domains. Results confirm the build up of local maxima and minima in the propagating particle front dynamics. The method of characteristics is shown to successfully predict particle motions and the position of the particle front, although it fails to accurately predict suspended particle concentrations in the vicinity of sharp gradients, such as at the particle front peak seen in some injection cases, where particle diffusion inevitably plays an important role. Results inform the design of applications in which the use of applied solute gradients can greatly enhance particle injection into and withdrawal from pores.

Diffusiophoretic manipulation of particles in a drop deposited on a hydrogel.

We report an experimental study on the manipulation of colloidal particles in a drop sitting on a hydrogel. The manipulation is achieved by diffusiophoresis, which describes a directed motion of particles induced by solute gradients. By letting the solute concentrations for the drop and the hydrogel be different, we control the motion of particles in a stable suspension, which is otherwise difficult to achieve. We show that diffusiophoresis can cause the particles to move either toward or away from the liquid-air interface depending on the direction of the solute gradient and the surface charge of the particles. We measure the particle adsorption experimentally and rationalize the results with a one-dimensional numerical model. We show that diffusiophoretic motion is significant at the lengthscale of a drop deposited on a hydrogel, which suggests a simple method for the deposition of particles on hydrogels.

Vortex-Breakdown-Induced Particle Capture in Branching Junctions.

We show experimentally that a flow-induced, Reynolds number-dependent particle-capture mechanism in branching junctions can be enhanced or eliminated by varying the junction angle. In addition, numerical simulations are used to show that the features responsible for this capture have the signatures of classical vortex breakdown, including an approach flow aligned with the vortex axis and a pocket of subcriticality. We show how these recirculation regions originate and evolve and suggest a physical mechanism for their formation. Furthermore, comparing experiments and numerical simulations, the presence of vortex breakdown is found to be an excellent predictor of particle capture. These results inform the design of systems in which suspended particle accumulation can be eliminated or maximized.

Flow-Driven Rapid Vesicle Fusion via Vortex Trapping.

Fusion between suspended lipid vesicles is difficult to achieve without membrane proteins or ions because the vesicles have extremely low equilibrium membrane tension and high poration energy. Nonetheless, vesicle fusion in the absence of mediators can also be achieved by mechanical forcing that is strong enough to induce membrane poration. Here, we employ a strong fluid shear stress to achieve vesicle fusion. By utilizing a unique vortex formation phenomenon in branched channels as a platform for capturing, stressing, and fusing the lipid vesicles, we directly visualize using high-speed imaging the vesicle fusion events, induced solely by shear, on the time scale of submilliseconds. We show that a large vesicle with a size of up to ∼10 µm can be achieved by the fusion of nanoscale vesicles. This technique has the potential to be utilized as a fast and simple way to produce giant unilamellar vesicles and to serve as a platform for visualizing vesicle interactions and fusions in the presence of shear.

The race of nanowires: morphological instabilities and a control strategy.

The incomplete growth of nanowires that are synthesized by template-assisted electrodeposition presents a major challenge for nanowire-based devices targeting energy and electronic applications. In template-assisted electrodeposition, the growth of nanowires in the pores of the template is complex and unstable. Here we show theoretically and experimentally that the dynamics of this process is diffusion-limited, which results in a morphological instability driven by a race among nanowires. Moreover, we use our findings to devise a method to control the growth instability. By introducing a temperature gradient across the porous template, we manipulate ion diffusion in the pores, so that we can reduce the growth instability. This strategy significantly increases the length of nanowires. In addition to shedding light on a key nanotechnology, our results may provide fundamental insights into a variety of interfacial growth processes in materials science such as crystal growth and tissue growth in scaffolds.

Diffusiophoresis promotes phase separation and transport of biomolecular condensates.

The internal microenvironment of a living cell is heterogeneous and comprises a multitude of organelles with distinct biochemistry. Amongst them are biomolecular condensates, which are membrane-less, phase-separated compartments enriched in system-specific proteins and nucleic acids. The heterogeneity of the cell engenders the presence of multiple spatiotemporal gradients in chemistry, charge, concentration, temperature, and pressure. Such thermodynamic gradients can lead to non-equilibrium driving forces for the formation and transport of biomolecular condensates. Here, we report how ion gradients impact the transport processes of biomolecular condensates on the mesoscale and biomolecules on the microscale. Utilizing a microfluidic platform, we demonstrate that the presence of ion concentration gradients can accelerate the transport of biomolecules, including nucleic acids and proteins, via diffusiophoresis. This hydrodynamic transport process allows localized enrichment of biomolecules, thereby promoting the location-specific formation of biomolecular condensates via phase separation. The ion gradients further impart active motility of condensates, allowing them to exhibit enhanced diffusion along the gradient. Coupled with a reentrant phase behavior, the gradient-induced active motility leads to a dynamical redistribution of condensates that ultimately extends their lifetime. Together, our results demonstrate diffusiophoresis as a non-equilibrium thermodynamic force that governs the formation and transport of biomolecular condensates.

Fluid Flow to Electricity: Capturing Flow-Induced Vibrations with Micro-Electromechanical-System-Based Piezoelectric Energy Harvester.

We introduce a micro-electromechanical system (MEMS) energy harvester, designed for capturing flow energy. Moving beyond traditional vibration-based energy harvesting, our approach incorporates a cylindrical oscillator mounted on an MEMS chip, effectively harnessing wind energy through flow-induced vibration (FIV). A highlight of our research is the development of a comprehensive fabrication process, utilizing a 5.00 µm thick cantilever beam and piezoelectric film, optimized through advanced micromachining techniques. This process ensures the harvester's alignment with theoretical predictions and enhances its operational efficiency. Our wind tunnel experiments confirmed the harvester's capability to generate a notable electrical output, with a peak voltage of 2.56 mV at an 8.00 m/s wind speed. Furthermore, we observed a strong correlation between the experimentally measured voltage frequencies and the lift force frequency observed by CFD analysis, with dominant frequencies identified in the range of 830 Hz to 867 Hz, demonstrating the potential application in actual flow environments. By demonstrating the feasibility of efficient energy conversion from ambient wind, our research contributes to the development of sustainable energy solutions and low-power wireless electron devices.

Directed colloidal assembly and banding via DC electrokinetics.

Manipulating the transport and assembly of colloidal particles to form segregated bands or ordered supracolloidal structures plays an important role in many aspects of science and technology, from understanding the origin of life to synthesizing new materials for next-generation manufacturing, electronics, and therapeutics. One commonly used method to direct colloidal transport and assembly is the application of electric fields, either AC or DC, due to its feasibility. However, as colloidal segregation and assembly both require active redistribution of colloidal particles across multiple length scales, it is not apparent at first sight how a DC electric field, either externally applied or internally induced, can lead to colloidal structuring. In this Perspective, we briefly review and highlight recent advances and standing challenges in colloidal transport and assembly enabled by DC electrokinetics.