Interface Dynamics at a Four-Fluid Interface during Droplet Impact on a Two-Fluid System.

We investigate the interfacial dynamics involved in the impact of a droplet on a liquid-liquid system, which involves the impingement of an immiscible core liquid drop from a vertical separation onto an interfacial shell liquid layer floating on a host liquid bath. The dynamics have been studied for a wide range of impact Weber numbers and two different interfacial shell liquids of varying volumes. The core drop, upon impact, dragged the interfacial liquid into the host liquid, forming an interfacial liquid column with an air cavity inside the host liquid bath. The dynamics is resolved into cavity expansion and rapid contraction, followed by thinning of the interfacial liquid. The interplay of viscous dissipation, interfacial pull, and core drop inertia influenced the necking dynamics. The viscous dissipation increases with the thickness of the interfacial layer, which depends on the volume and lateral spread over the water. The necking dynamics transitioned from inertia-dominated deep seal closure at higher spread, lower interfacial film volumes, and higher Weber numbers into inertia-capillary-dominated deep seal closure with an increase in film volumes, decrease in the spread of the interfacial fluid, or decrease in Weber number and finally into a no-seal closure at high volumes, low spread, and low Weber numbers.

Bacteria-surface interactions: role of impacting bacteria-laden droplets.

Understanding the interactions of pathogenic droplets with surfaces is crucial to biomedical applications. In this study, using E. coli as the model microbe, we investigate the impact of a bacteria-laden droplet on different substrates, both bare and antimicrobial. In doing so, we unveil the significance of kinetic energy and spreading parameters of the impacting droplet in determining the microbes' proliferation capabilities. Our results indicate an inverse relationship between the impact Weber number and the bacterial ability to proliferate. We reveal that the mechanical stress generated during impact impedes the capabilities of microbes present inside the droplet to create their progeny. Following an order analysis of the mechanical stress generated, we argue that the impact does not induce lysis-driven cell death of the bacteria; rather, it promotes a stress-driven transition of viable bacteria to a viable-but-non-culturable (VBNC) state. Furthermore, variations in the concentration of particles on the antimicrobial surfaces revealed the role of the post-impact spreading behaviour in dictating bacterial proliferation capabilities. Contrary to the conventional notion, we demonstrate that during the early stages of interaction, a bare substrate may outperform an antibacterial substrate in the inactivation of the bacterial load. Finally, we present an interaction map illustrating the complex relationship between bacterial colony-forming units, bactericide concentration on the surface, and the impact Weber number. We believe that the inferences of the study, highlighting the effect of mechanical stresses on the soft cell wall of microbes, could be a useful design consideration for the development of antimicrobial surfaces.

Probing Liquid Drop Induced Deformation on Soft Solids Using Dual-Wavelength Reflection Interference Contrast Microscopy.

A liquid drop resting on a soft solid deforms the surface at the three-phase contact line. The surface deformation, also called "wetting ridge", varies in size from nanoscales to microscales, depending on the elasticity and thickness of the soft layer. In this work, we probe how surface elasticity and coating thickness influences normal and tangential surface deformation profiles induced by a sessile liquid drop using dual-wavelength reflection interference contrast microscopy. Furthermore, we experimentally verify the appropriate characteristic length scale, which closely describes the ridge profiles on both thick and thin soft layers for two different surface elasticities.

Microparticle Suspensions and Bacteria-Laden Droplets: Are They the Same in Terms of Wetting Signature?

Adhesion behavior of microbial pathogens on commonly encountered surfaces is one of the most pertinent questions now. We present the characterization of bacteria-laden droplets and quantify the adhesion forces on highly repellent surfaces with the help of a simple experimental setup. Comparing the force signature measured directly using an in-house capillary deflection-based droplet force apparatus, we report an anomalous adhesion behavior of live bacteria (E. coli)-laden droplets on repellent surfaces, which stands in stark contrast to the observed adhesion signature when the doping agent is changed to inert microparticles or the same bacteria in an incapacitated state. We showed that the regular contact angle measurements using optical goniometry is unable to differentiate between the live bacteria and the dead ones (including microparticles) and thus delineate its limitations and the complementary nature of the adhesion measurements in understanding the fundamental interfacial interaction of living organisms on solid surfaces.

Reflected Laser Interferometry: A Versatile Tool to Probe Condensation of Low-Surface-Tension Droplets.

Experimental investigation of dropwise condensation of low-surface-tension liquids remains prone to error owing to the imaging difficulties caused by the typically low droplet height. Using reflection interference contrast microscopy in confocal mode, we demonstrate a noninvasive framework to accurately capture this condensation dynamics of volatile liquids with low surface tension. The capability of the developed framework is demonstrated in studying the condensation dynamics of acetone, where it accurately describes the growth mechanism of condensed microdroplets with excellent spatiotemporal resolution even for submicron-range drop height and a three-phase contact angle of <5°. From experimentally obtained interferograms, the framework can reconstruct three-dimensional topography of the microdroplets even when the contact line of the droplet is distorted due to strong local pinning. The obtained results exhibit excellent quantitative agreement with several theoretically predicted trends. The proposed protocol overcomes the limitation of conventional techniques (e.g., optical imaging/environmental scanning electron microscopy) and provides an efficient alternative for studying the condensation of low-surface-tension liquids under atmospheric conditions.

Precursor-Film-Mediated Thermocapillary Motion of Low-Surface-Tension Microdroplets.

In contrast to microdroplet condensation with high contact angles, the one with low contact angles remains unclear. In this study, we investigated dynamics of microdroplet condensation of low-surface-tension liquids on two flat substrate surfaces by using reflection interference confocal microscopy. Spontaneous migration toward relatively larger droplets was first observed for the microdroplets nucleated on the hydrophilic quartz surface. The moving microdroplets showed a contact angle hysteresis of ∼0.5°, which is much lower than the values observed on typical flat substrates and is within the range observed on slippery lubricant-infused porous surfaces. Because the microdroplets on the hydrophobic polydimethylsiloxane surface did not move, we concluded that the ultrathin precursor film is formed only on the hydrophilic surface, which reduces a resistive force to migration. Also, reduced size of droplets promotes the thermocapillary motion, which is induced by a gradient in local temperature inside a small microdroplet arising due to the difference in size of adjacent droplets.

Friction and Adhesion of Microparticle Suspensions on Repellent Surfaces.

With the recent advancements in the development and application of repellent surfaces, both in air and under liquid medium, accurate characterization of repellence behavior is critical in understanding the mechanism behind many observed phenomena and to exploit them for novel applications. Conventionally, the repellence behavior of a surface is characterized by the optical measurement of the dynamic contact angle of the target (to be repelled) liquid on the test surface. However, as already established in the literature, optical measurements are prone to appreciable error, especially for repellent surfaces with high contact angles. Here, we present an alternative, more accurate force-based characterization method of both friction and adhesion forces of microparticle-laden aqueous droplets over various repellent surfaces, where the force signature is captured by probing the surface with a droplet of the test liquid mounted at the tip of a flexible cantilever and then tracking the deflection of the tip of the cantilever as the probe droplet interacts with the surface. A systematic investigation of the response of repellent surfaces toward droplets with different microparticle concentrations reveals the dependency and sensitivity of measured adhesion and friction signature toward particle concentration. A comparison with the theoretical estimate from optical goniometry highlights the deviation of the theoretical data from experimentally measured values and further substantiates the need for such a force-based approach for accurate characterization of repellence behavior.

A universal capillary-deflection based adhesion measurement technique.

HYPOTHESIS: Contact angle goniometry suffers from inherent optical challenges such as scattering and diffraction near the triple contact line (TCL) rendering erroneous results. Alternatively, the cantilever-based direct adhesion measurement was constrained to low-energy surfaces to date due to the inability of the probe droplet to retract (pull-off) from high-energy surfaces completely. The present study revisits the cantilever approach from a fundamental physical perspective and generalizes the approach to render it wettability invariant. EXPERIMENTS: The adhesive wetting interaction between a probe droplet (attached to a cantilever) with the test substrate is recorded with a high-speed camera. Image processing and subsequent motion analysis enable us to accurately calculate the adhesion force (in the sub-micron range) exhibited by the test substrate. FINDINGS: We experimentally demonstrate the contact line depinning (and not the droplet pull-off) to be the only prerequisite for accurately quantifying the characteristic adhesion force. We alsoreveal that depinning precedes the onset of cantilever retraction due to the inertia effect. Further, we establish that the characteristic adhesion corresponds to zero acceleration of the cantilever and not to its maximum deflection. The inferences of the study will be beneficial in the rational design of direct wetting characterization methods for any substrate.

Liquid-Liquid Encapsulation: Penetration vs. Trapping at a Liquid Interfacial Layer.

Encapsulation protects vulnerable cores in an aggressive environment and imparts desirable functionalities to the overall encapsulated cargo, including control of mechanical properties, release kinetics, and targeted delivery. Liquid-liquid encapsulation to create such capsules, where a liquid layer (shell) is used to wrap another liquid (core), is an attractive value proposition for ultrafast encapsulation (∼100 ms). Here, we demonstrate a robust framework for stable liquid-liquid encapsulation. Wrapping is achieved by simple impingement of a target core (in liquid form) on top of an interfacial layer of another shell-forming liquid floating on a host liquid bath. Poly(dimethylsiloxane) (PDMS) is chosen as the shell-forming liquid due to its biocompatibility, physicochemical stability, heat curability, and acceptability as both a drug excipient and food additive. Depending on the kinetic energy of the impinging core droplet, encapsulation is accomplished by either of the two pathways─necking-driven complete interfacial penetration and subsequent generation of encapsulated droplets inside the host bath or trapping inside the interfacial layer. Combining thermodynamic argument with experimental demonstration, we show that the interfacially trapped state, which results in a low kinetic energy of impact, is also an encapsulated state where the core droplet is wholly enclosed inside the floating interfacial layer. Therefore, despite being impact-driven, our method remains kinetic energy independent and minimally restrictive. We describe the underlying interfacial evolution behind encapsulation and experimentally identify a nondimensional regime of occurrence for the two pathways mentioned above. Successful encapsulation by either path offers efficient long-term protection of the encased cores in aggressive surroundings (e.g., protection of honey/maple syrup inside a water bath despite their miscibility). We enable the generation of multifunctional compound droplets via interfacial trapping, where multiple core droplets with different compositions are encapsulated within the same wrapping shell. Further, we demonstrate the practical utility of the interfacially trapped state by showing successful heat-curing of the shell and subsequent extraction of the capsule. The cured capsules are sufficiently robust and remain stable under normal handling.

Bioinspired Scalable Lubricated Bicontinuous Porous Composites with Self-Recoverability and Exceptional Outdoor Durability.

Lubricant-impregnated surfaces (LIS) are promising as efficient liquid-repellent surfaces, which comprise a surface lubricant layer stabilized by base solid structures. However, the lubricant layer is susceptible to depletion upon exposure to degrading stimuli, leading to the loss of functionality. Lubricant depletion becomes even more pronounced in exposed outdoor conditions, restricting LIS to short-term lab-scale applications. Thus, the development of scalable and long-term stable LIS suitable for practical outdoor applications remains challenging. In this work, we designed "Lubricated Bicontinuous porous Composites" (LuBiCs) by infusing a silicone oil lubricant into a bicontinuous porous composite matrix of tetrapod-shaped zinc oxide microfillers and poly(dimethylsiloxane). LuBiCs are prepared in the meter scale by a facile drop-casting inspired wet process. The bicontinuous porous feature of the LuBiCs enables capillarity-driven spontaneous lubricant transport throughout the surface without any external driving force. Consequently, the LuBiCs can regain liquid-repellent function upon lubricant depletion via capillary replenishment from a small, connected lubricant reservoir, making them tolerant to lubricant-degrading stimuli (e.g., rain shower, surface wiping, and shearing). As a proof-of-concept, we show that the large-scale "LuBiC roof" retains slippery behavior even after more than 9 months of outdoor exposure.

Quantifying Water Friction in Misaligned Graphene Channels under Ångström Confinements.

Two-dimensional (2D) materials, such as graphene (GE), hold great potential to be employed as the fundamental building blocks of novel nanofluidic devices for a wide range of applications. Recent advances in experimental techniques are materializing such prospects by enabling the assembly of 2D material-based fluidic channels with heights as small as few Ångströms. Here, we conduct molecular dynamics simulations to probe the effect of the relative misalignment between the walls of the GE fluidic channel with Ångströms height on the resistance to water transport through the channel. Two types of misalignments are studied, namely, translational and rotational misalignments. Our results show that the relative misalignment of the GE lattices can lead to a substantial reduction in the friction between water and the channel walls. Moreover, a dependence of the friction on the degree of misalignment and flow direction is found for the cases with translational misalignment. In contrast, the resistance exerted by the channels with rotational misalignment is found to be independent of the rotation angle (θ) for 0° < θ < 60° but always lower than the perfectly aligned case. We associate such lowering of the resistance to water transport to the corrugation and the anisotropy in the corresponding potential energy landscape associated with each degree of misalignment. The findings, therefore, point to an unprecedented possibility of significantly enhancing the water transport in Ångströms height GE channels by engineering the misalignments of the GE channel walls.

Encapsulation with an interfacial liquid layer: Robust and efficient liquid-liquid wrapping.

HYPOTHESIS: We developed an impact driven liquid-based encapsulation method by utilizing the fundamental thermodynamic tendency of a suitable three-liquid combination towards formation of a core-shell structure. EXPERIMENTS: Stable wrapping is achieved by impinging a core drop from a vertical separation on an interfacial liquid film floating on a host liquid bath. The resulting interfacial dynamics is captured using a high-speed camera. Several combinations of impact height and interfacial film thickness are investigated for a quantitative description of the phenomena. FINDINGS: The stability and integrity of the liquid encapsulating layer are confirmed both experimentally (by analyzing the under-liquid wetting signature) and theoretically (by equilibrium thermodynamic analysis). Effect of viscous dissipation on the dynamics is explained and a consequent theoretical threshold for minimum allowable drop size is provided. A non-dimensional experimental regime is also constructed for successful encapsulation in terms of impact kinetic energy and interfacial layer thickness. Additionally, the encapsulating layer is shown to protect the core drop even when the core and host liquids are miscible. The demonstrated method is simple to implement yet robust, offers flexibility regarding varying both the size and the material properties of the core and shell liquids and consistently produces stable monodispersed encapsulated drops in an ultrafast manner.