Self-Lifting Droplet Driven by the Solidification-Induced Solutal Marangoni Flow.

Multicomponent droplets are pertinent to diverse applications ranging from 3D printing to fabrication of electronic devices to medical diagnostics and are typically inherent with the occurrence of the phase transition in the manifestation of evaporation and solidification. Indeed, the versatile transformations and fascinating morphologies of the droplets have been identified, which primarily arise from the evaporation-induced flow. Here, we report the self-lifting behavior of a frozen binary droplet, resulting in a nearly doubling in height, in a fashion that defies against the gravitational effect. This counterintuitive observation is attributed to an internal solutal Marangoni flow up to 1 mm/s, which is driven by the enriched solute concentration locally in the vicinity of the solidification front. Moreover, we perform theoretical analysis by incorporating the propagation of solidification front, and the calculated spatiotemporal evolution of droplet shape agrees with experiments excellently. The effects of several key physical parameters on self-lifting are elucidated quantitatively, providing guidance to control the self-lifting. These results will further advance our understanding of underlying physicochemical hydrodynamics in the multicomponent liquid systems subjected to heat transfer and phase change, consequently shedding light on the relevant technological applications.

Controlled filamentation instability as a scalable fabrication approach to flexible metamaterials.

Long and flexible arrays of nanowires find impactful applications in sensing, photonics, and energy harvesting. Conventional manufacturing relies largely on lithographic methods limited in wafer size, rigidity, and machine write time. Here, we report a scalable process to generate encapsulated flexible nanowire arrays with high aspect ratios and excellent tunable size and periodicity. Our strategy is to control nanowire self-assembly into 2D and 3D architectures via the filamentation of a textured thin film under anisotropic stretching. This is achieved by coupling soft lithography, glancing angle deposition, and thermal drawing to obtain well-ordered meters-long nanowires with diameters down to 50 nanometers. We demonstrate that the nanowire diameter and period of the array can be decoupled and manipulated independently. We propose a filamentation criterion and perform numerical simulations implementing destabilizing long-range Van der Waals interactions. Applied to high-index chalcogenide glasses, we show that this decoupling allows for tuning diffraction. Finally, harnessing Mie resonance, we demonstrate the possibility of manufacturing macroscopic meta-grating superstructures for nanophotonic applications.

Near-infrared-laser-navigated dancing bubble within water via a thermally conductive interface.

Precise manipulation of droplets or bubbles hosts a broad range of applications for microfluidic devices, drug delivery, and soft robotics. Generally the existing approaches via passively designing structured surfaces or actively applying external stimuli, inherently confine their motions within the planar or curved geometry at a slow speed. Consequently the realization of 3D manipulation, such as of the underwater bubbles, remains challenging. Here, during the near-infrared-laser impacting on water, by simply introducing a thermally conductive interface, we unexpectedly observe a spontaneously bouncing bubble with hundreds-of-micrometer diameter at tens-of-Hertz frequency. The unique formation of temperature inversion layer in our system generates the depth-dependent thermal Marangoni force responsible for the bouncing behavior. Both the scaling analysis and numerical simulation agree with observations quantitatively. Furthermore, by controlling the navigation speed of the laser beam, the bubble not only shows excellent steerability with velocity up to 40 mm/s, but also exhibits distinctive behaviors from bouncing to dancing within water. We demonstrate the potential applications by steering the bubble within water to specifically interact with tiny objects, shedding light on the fabrication of bubble-based compositions in materials science and contamination removal in water treatment.

Observation of Remote Electroconvection and Inert-Cation Concentration Valley within Supporting Electrolytes in a Microfluidic-Based Electrochemical Device.

The electrochemical system is playing an increasingly important role in the advanced technology development for drinkable water and energy storage. While the binary electrolyte has been widely studied, such as the associated intriguing interfacial instabilities, multi-component electrolyte is by far less known. Here, based on the classic Cu|CuSO4 |Cu electrochemical system, the effect of supporting electrolyte is systematically investigated by highlighting the inert cations. In an annulus microfluidic device, the suppression of a previously known electro-osmotic instability and the emergence of an array of the remote electroconvection along the azimuthal direction is found. A distinctive inert-cation concentration valley propagates radially outward at a speed limited by the electromigration velocity. Remarkably, the simultaneous visualization of spatiotemporal evolution demonstrates the correlation of the concentration valley and electroconvection at a microscopic level. The underlying physical mechanism of their correlation is discussed, and the scaling analysis agrees with experiments. This work might inspire more future work on the multi-component electrolyte, such as for the suppression of interfacial hydrodynamic instability and mitigation of dendrite growth, with the technological implications for water treatment and energy storage in batteries.

Nanoparticle-Mediated Cavitation via CO2 Laser Impacting on Water: Concentration Effect, Temperature Visualization, and Core-Shell Structures.

By taking advantage of seeded polymer nanoparticles and strong photo energy absorption, we report CO2 laser impacting on water to produce cavitation at the air/water interface. Using a high-speed camera, three regimes (no cavitation, cavitation, and pseudo-cavitation) are identified within a broad range of nanoparticles concentration and size. The underlying correlation among cavitation, nanoparticles and temperature is revealed by the direct observation of spatiotemporal evolution of temperature using a thermal cameral. These findings indicate that nanoparticles not only act as preexisted nuclei to promote nucleation for cavitation, but also likely affect temperature to change the nucleation rate as well. Moreover, by exploiting a compound hexane/water interface, a novel core-shell cavitation is demonstrated. This approach might be utilized to attain and control cavitations by choosing nanoparticles and designing interfaces while operating at a lower laser intensity, for versatile technological applications in material science and medical surgery.

Overlimiting current and shock electrodialysis in porous media.

Most electrochemical processes, such as electrodialysis, are limited by diffusion, but in porous media, surface conduction and electroosmotic flow also contribute to ionic flux. In this article, we report experimental evidence for surface-driven overlimiting current (faster than diffusion) and deionization shocks (propagating salt removal) in a porous medium. The apparatus consists of a silica glass frit (1 mm thick with a 500 nm mean pore size) in an aqueous electrolyte (CuSO4 or AgNO3) passing ionic current from a reservoir to a cation-selective membrane (Nafion). The current-voltage relation of the whole system is consistent with a proposed theory based on the electroosmotic flow mechanism over a broad range of reservoir salt concentrations (0.1 mM to 1.0 M) after accounting for (Cu) electrode polarization and pH-regulated silica charge. Above the limiting current, deionized water (≈10 µM) can be continuously extracted from the frit, which implies the existence of a stable shock propagating against the flow, bordering a depleted region that extends more than 0.5 mm across the outlet. The results suggest the feasibility of shock electrodialysis as a new approach to water desalination and other electrochemical separations.

Structured spheres generated by an in-fibre fluid instability.

From drug delivery to chemical and biological catalysis and cosmetics, the need for efficient fabrication pathways for particles over a wide range of sizes, from a variety of materials, and in many different structures has been well established. Here we harness the inherent scalability of fibre production and an in-fibre Plateau-Rayleigh capillary instability for the fabrication of uniformly sized, structured spherical particles spanning an exceptionally wide range of sizes: from 2 mm down to 20 nm. Thermal processing of a multimaterial fibre controllably induces the instability, resulting in a well-ordered, oriented emulsion in three dimensions. The fibre core and cladding correspond to the dispersed and continuous phases, respectively, and are both frozen in situ on cooling, after which the particles are released when needed. By arranging a variety of structures and materials in a macroscopic scaled-up model of the fibre, we produce composite, structured, spherical particles, such as core-shell particles, two-compartment 'Janus' particles, and multi-sectioned 'beach ball' particles. Moreover, producing fibres with a high density of cores allows for an unprecedented level of parallelization. In principle, 10(8) 50-nm cores may be embedded in metres-long, 1-mm-diameter fibre, which can be induced to break up simultaneously throughout its length, into uniformly sized, structured spheres.

Thermal drawing of high-density macroscopic arrays of well-ordered sub-5-nm-diameter nanowires.

We investigate the lower limit of nanowire diameters stably produced by the process of thermal fiber drawing and fiber tapering. A centimeter-scale macroscopic cylindrical preform containing the nanowire material in the core encased in a polymer scaffold cladding is thermally drawn in the viscous state to a fiber. By cascading several iterations of the process, continuous reduction of the diameter of an amorphous semiconducting chalcogenide glass is demonstrated. Starting from a 10-mm-diameter rod we thermally draw hundreds of meters of continuous sub-5-nm-diameter nanowires. Using this approach, we produce macroscopic lengths of high-density, well-ordered, globally oriented nanowire arrays.