New insights and novel perspectives in bileaflet mechanical heart valve prostheses thromboresistance.

BACKGROUND: Although well-known for their thromboresistance, bileaflet mechanical heart valves (BMHV) require lifelong anti-thrombotic therapy. This must be associated with a certain level of thrombogenicity. Since both thromboresistance and thrombogenicity are explained by the blood-artificial surface or liquid-solid interactions, the aim of the present study was to explore BMHV thromboresistance from new perspectives. The wettability of BMHV pyrolytic carbon (PyC) occluders was investigated in under-liquid conditions. The submerged BMHV wettability clarifies the mechanisms involved in the thromboresistance. METHODS: The PyC occluders of a SJM Regent™ BMHV were previously laser irradiated, to create a surface hierarchical nano-texture, featuring three nano-configurations. Additionally, four PyC occluders of standard BMHV (Carbomedics, SJM Regent™, Bicarbon™, On-X®), were investigated. All occluders were evaluated in under-liquid configuration, with silicon oil used as the working droplet, while water, simulating blood, was used as the surrounding liquid. The under-liquid droplet-substrate wetting interactions were analyzed using contact angle goniometry. RESULTS: All the standard occluders showed very low contact angle, reflecting a pronounced affinity for non-polar molecules. No receding of the contact line could be observed for the untreated occluders. The smallest static contact angle of around 61° could be observed for On-X® valve (the only valve made of full PyC). The laser-treated occluders strongly repelled oil in underwater conditions. A drastic change in their wetting behaviour was observed depending on the surrounding fluid, displaying a hydrophobic behaviour in the presence of air (as the surrounding medium), and showing instead a hydrophilic nature, when surrounded by water. CONCLUSIONS: BMHV "fear" water and blood. The intrinsic affinity of BMHV for nonpolar fluids can be translated into a tendency to repel polar fluids, such as water and blood. The blood-artificial surface interaction in BMHV is minimized. The contact between blood and BMHV surface is drastically reduced by polar-nonpolar Van der Waals forces. The "hydro/bloodphobia" of BMHV is intrinsically related to their chemical composition and their surface energy, thus their material: PyC indeed. Pertaining to thromboresistance, the surface roughness does not play a significant role. Instead, the thromboresistance of BMHV lies in molecular interactions. BMHV wettability can be tuned by altering the surface interface, by means of nanotechnology.

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.

Flexible hydrogels connecting adhesion and wetting.

Raindrops falling on window-panes spread upon contact, whereas hail can cause dents or scratches on the same glass window upon contact. While the former phenomenon resembles classical wetting, the latter is dictated by contact and adhesion theories. The classical Young-Dupre law applies to the wetting of pure liquids on rigid solids, whereas conventional contact mechanics theories account for rigid-on-soft or soft-on-rigid contacts with small deformations in the elastic limit. However, the crossover between adhesion and wetting is yet to be fully resolved. The key lies in the study of soft-on-soft interactions with material properties intermediate between liquids and solids. In this work, we translate adhesion to wetting by experimentally probing the static signature of hydrogels in contact with soft PDMS of varying elasticity of both the components. Consequently, we probe this transition across six orders of magnitude in terms of the characteristic elasto-adhesive parameter of the system. In doing so, we reveal previously unknown phenomenology and a theoretical model which smoothly bridges adhesion of glass spheres with total wetting of pure liquids on any given substrate.

Density Functional Theory Approach to Interpret Elastowetting of Hydrogels.

Sessile hydrogel drops on rigid surfaces exhibit a wetting/contact morphology intermediate between liquid drops and glass spheres. Using density functional theory, we reveal the contact forces acting between a hydrogel and a rigid glass surface. We show that while transitioning from liquid-like to solid-like hydrogels, there exists a critical hydrogel elasticity that enables a switch from attractive-to-repulsive interaction with the underlying rigid glass surface. Our theoretical model is validated by experimental observations of sessile polyacrylamide hydrogels of varying elasticity on glass surfaces. Further, the proposed model successfully approaches Young's law in the pure liquid limit and work of adhesion in the glassy limit. Lastly, we show a modified contact angle relation, taking into account the hydrogel elasticity to explain the features of a distinct hydrogel foot.

Cs+ conductance in graphene membranes with Ångström-scale pores: the role of pore entrance geometry.

Recently, 2D materials, such as graphene, have been successfully implemented as artificial conduits of molecular sizes. The extreme precision with which these structures can be fabricated provides an unprecedented framework for the development of highly specific and efficient devices. In this work, we study the electrophoretic transport of Cs+ ions in a graphene membrane with effective pore heights of 3.4 Å by conducting molecular dynamics simulations. The entrance of the pore is systematically modified to investigate the effect of pore geometry on ionic conductance. Simulation results suggest a significant correlation between ionic conductance and entrance geometry, with a variation of the conductance up to 100% across the studied cases. To explain the observed correlation, two mechanisms involving an intimate relationship between ion dehydration and edge functional groups are proposed. The present study provides theoretical insights that can aid the design of graphene-based membranes with tunable ionic transport properties.

Directional Manipulation of Drops and Solids on a Magneto-Responsive Slippery Surface.

The cloaking of the droplet and solid spheres by a thin ferrofluid layer forms a ferrofluid-wetting ridge, enabling the magnet-assisted directional manipulation of droplets and solid spheres on the magneto-responsive slippery surface. Understanding the interplay of various forces governing motion unravels the manipulation mechanism. The transportation characteristics of droplets and solid spheres on such surfaces enable their controlled manipulation in multiple applications. Here, we prepare magneto-responsive slippery surfaces by using superhydrophobic coatings on glass slides, creating a porous network and impregnating them with ferrofluid. Using a permanent magnet (and its translation) in the proximity of these surfaces, we manipulate the motion of liquid drops and solid spheres. Upon dispensing the droplet on the magneto-responsive slippery surface, the droplet is cloaked by a thin ferrofluid layer and forms a ferrofluid wetting ridge. Incorporating the magnetic field creates a magnetic-nanoparticle-rich zone surrounding the ferrofluid ridge. Thereafter, the motion of the magnet gives rise to the movement of the droplet. We found that the interplay of the magnetic force and viscous drag leads to the magnetic manipulation of droplets in a controlled fashion up to a certain magnet speed. Increasing the magnet speed further results in the uncontrolled motion of the droplet, where the droplet cannot follow the magnet trajectory. Moreover, we delineate multifunctional droplet manipulations, such as trapping, pendant droplet manipulation, coalescence, and microchemical reactions, which have wide engineering applications.

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.

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.

Magnetic Control of Water Droplet Impact onto Ferrofluid Lubricated Surfaces.

Controlling the impact process of a droplet impacting a liquid film has remained a wide-open challenge. The existing passive techniques lack precise on-demand control of the impact dynamics of droplets. The present study introduces a magnet-assisted approach to control water droplets' impact dynamics. We show that by incorporating a thin, magnetically active ferrofluid film, the overall droplet impact phenomena of the water droplets could be controlled. It is found that by modifying the distribution of the magnetic nanoparticles (MNPs) present inside the ferrofluid using a permanent magnet, the spreading and retraction behavior of the droplet could be significantly controlled. In addition to that, we also show that by altering the impact Weber number (Wei), and the magnetic Bond number (Bom), the outcomes of droplet impact could be precisely controlled. We reveal the role of the various forces on the consequential effects of droplet impact with the help of phase maps. Without the magnetic field, we discovered that the droplet impact on ferrofluid film results in no-splitting, jetting, and splashing regimes. On the other hand, the presence of magnetic field results in the no-splitting and jetting regime. However, beyond a critical magnetic field, the ferrofluid film gets transformed into an assembly of spikes. In such scenarios, the droplet impact only results in no-splitting and splashing regimes, while the jetting regime remains absent. The outcome of our study may find potential applications in chemical engineering, material synthesis, and three-dimensional (3D) printing where the control and optimization of the droplet impact process are desirable.

Recent advances in label-free optical, electrochemical, and electronic biosensors for glioma biomarkers.

Gliomas are the most commonly occurring primary brain tumor with poor prognosis and high mortality rate. Currently, the diagnostic and monitoring options for glioma mainly revolve around imaging techniques, which often provide limited information and require supervisory expertise. Liquid biopsy is a great alternative or complementary monitoring protocol that can be implemented along with other standard diagnosis protocols. However, standard detection schemes for sampling and monitoring biomarkers in different biological fluids lack the necessary sensitivity and ability for real-time analysis. Lately, biosensor-based diagnostic and monitoring technology has attracted significant attention due to several advantageous features, including high sensitivity and specificity, high-throughput analysis, minimally invasive, and multiplexing ability. In this review article, we have focused our attention on glioma and presented a literature survey summarizing the diagnostic, prognostic, and predictive biomarkers associated with glioma. Further, we discussed different biosensory approaches reported to date for the detection of specific glioma biomarkers. Current biosensors demonstrate high sensitivity and specificity, which can be used for point-of-care devices or liquid biopsies. However, for real clinical applications, these biosensors lack high-throughput and multiplexed analysis, which can be achieved via integration with microfluidic systems. We shared our perspective on the current state-of-the-art different biosensor-based diagnostic and monitoring technologies reported and the future research scopes. To the best of our knowledge, this is the first review focusing on biosensors for glioma detection, and it is anticipated that the review will offer a new pathway for the development of such biosensors and related diagnostic platforms.

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.

Capillary pressure mediated long-term dynamics of thin soft films.

HYPOTHESIS: The conventional solid-solid contact is well studied in the literature. However, a number of practical applications, such as adhesive patches and biomimetic surfaces, require a much deeper understanding of soft contact where there is a distinct time-dependent adhesion behavior due to the dual-phase structure (solids and liquids). To understand this, currently existing solid-solid contact behavior is extrapolated to soft contact, wherein the size-effect of the gel film and the preload are typically neglected. When introducing the finite-size effect and preload, gels could experience distinctive long-term contact dynamics in contact with another material. EXPERIMENTS: We reconstruct the evolving surface profile of the gel films intercalated between a glass sphere and glass slide using dual wavelength-reflection interference contrast microscopy. The macro-sized glass sphere compresses the gel. The indentation depth is comparable to the gel film thickness, wherein the conventional contact theories are inapplicable. FINDINGS: The gel surface experiences two deformation stages. The natural preload and elastic force develop the contact area in the early state. In the later state, the viscous free molecules of the gel develop the ridge. We discover that the residual surface stress relaxes over 85 hr. Our findings on the long-term gel deformation provide a new perspective on soft adhesion, from developing soft adhesives to understanding biological tissues.

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.

Toward Unveiling the Anomalies Associated with the Spontaneous Spreading of Droplets.

The liquid droplet spreads over a solid surface to minimize the surface energy when brought in direct contact with the surface. The spreading process is rapid in the early stages, tends to slow down during its progress, and has resulted in peculiarity due to the experimental difficulties in the accurate determination of the contact line radius. In the present numerical study, we found that drop spreading begins with a viscosity-dominated Stokes regime, where contact radius scales as r ∼ t for a wide range of drop liquid viscosities. Subsequent to the Stokes regime, the inertial regime is observed where contact radius scales as r ∼ t0.5 for low- to medium-viscous droplets, whereas for very high viscous drops, the spreading dynamics is completely dominated by the viscous regime. It is also found that the equilibrium wetting condition does not affect the power-law scaling for the contact radius of the drop. The amplitude of capillary waves induced across the interface of the drop is observed to be sufficiently high to cause necking and ejection of satellite drops from the main drop during its spreading for low-viscous liquids from complete wetting to partial wetting conditions. A regime plot between the Ohnesorge number and advancing contact angle of the substrate is presented to demarcate the regions of damped waves without pinch-off and drop spreading with satellite drops.

A novel method for fabrication of paper-based microfluidic devices using BSA-ink.

This paper describes the fabrication of paper-based microfluidic devices using a novel, inexpensive ink composed of bovine serum albumin (BSA), utilizing BSA's thermal denaturation and aggregation to create a hydrophobic barrier on Whatman® Grade 4 filter paper. A 20% aqueous solution of BSA was inked onto the paper using a pen plotter at moderate speed (5 cm/s) with desired shape and size followed by heating at 80 °C to denature the BSA leading to hydrophobic barriers formation, whereas below 80 °C the barrier layer is prone to collapse. The minimum line gap and line width of ~1 mm and ~1.3 mm were achieved. Finally, a proof-of-concept glucose sensing was shown while addressing the issue of the coffee ring effect using the biopolymer NanoCheck-ATH® from ChitoLytic Inc. The glucose concentration limit of detection (LOD) as low as 0.2 mg/mL was estimated. The developed technique offers ease of fabrication, high reproducibility, cost-effectiveness, and is environmentally friendly.

Reduced Pressure Drop in Viscoelastic Polydimethylsiloxane Wall Channels.

Polydimethylsiloxane (PDMS) is an important viscoelastic material that finds applications in a large number of engineering systems, particularly lab-on-chip microfluidic devices built with a flexible substrate. Channels made of PDMS, used for transporting analytes, are integral to these applications. The PDMS viscoelastic nature can induce additional hydrodynamic contributions at the soft wall/fluid interface compared to rigid walls. In this research, we investigated the pressure drop within PDMS channels bounded by rigid tubes (cellulose tubes). The bulging effect of the PDMS was limited by the rigid tubes under flowing fluids. The PDMS viscoelasticity was modulated by changing the ratio of the base to the cross-linker from 10:1 to 35:1. We observed that the pressure drop of the flowing fluids within the channel decreased with the increased loss tangent of the PDMS in the examined laminar regime [Reynolds number (Re) ∼ 23-58.6 for water and Re ∼ 0.69-8.69 for glycerol solution]. The elastic PDMS 10:1 wall channels followed the classical Hagen Poiseuille's equation, but the PDMS walls with lower cross-linker concentrations and thicker walls decreased pressure drops. The friction factor (f) for the PDMS channels with the two working fluids could be approximated as f = 47/Re. We provide a correlation between the pressure drop and PDMS viscoelasticity based on experimental findings. In the correlation, the loss tangent predominates; the larger the loss tangent, the smaller is the pressure drop. The research findings appear to be unexpected if only considering the energy dissipation of viscoelastic PDMS walls. We attributed the reduction in the pressure drop to a lubricating effect of the viscoelastic PDMS walls in the presence of the working fluids. Our results reveal the importance of the subtle diffusion of the residual oligomers and water from the bulk to the soft wall/fluid interface for the observed pressure drop in soft wall channels.

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.

Synthesis of Shape-Controllable Anisotropic Microparticles and "Walnut-like" Microparticles via Emulsion Interfacial Polymerization.

Anisotropic microparticles have plenty of applications for their asymmetric structure and precisely modified surface. In our research, the uniform anisotropic microparticles with benzyl chloride group were synthesized successfully via emulsion interfacial polymerization. By varying the degree of cross-linking and the concentration of slightly hydrophilic monomer 4-vinyl benzyl chloride (VBC), several types of microparticles with different concavities and different shapes of microparticles (hemisphere, bowl-like, egg-like, etc.) were obtained. Nanoporous microparticles with a walnut-like heterostructure were achieved with modified hydrophilic seeds with the same strategy. The potential applications of shape-controllable fluorescent microparticles and surface modification of microparticles by thiol-click reaction were explored. The modified microparticles achieved in this study are very useful in labeling, tracing, protein separation, and other biomedical fields.

Wetting, Adhesion, and Droplet Impact on Face Masks.

In the present pandemic time, face masks are found to be the most effective strategy against the spread of the virus within the community. As aerosol-based spreading of the virus is considered as the primary mode of transmission, the interaction of masks with incoming droplets needs to be understood thoroughly for an effective usage among the public. In the present work, we explore the interactions of the droplets over the most commonly used 3-ply surgical masks. A detailed study of the wetting signature, adhesion, and impact dynamics of water droplets and microbe-laden droplets is carried out for both sides of the mask. We found that the interfacial characteristics of the incoming droplets with the mask are very similar for the front and the back side of the mask. Further, in an anticipated attempt to reduce the adhesion, we have tested masks with a superhydrophobic coating. It is found that a superhydrophobic coating may not be the best choice for a regular mask as it can give rise to a number of smaller daughter droplets that can linger in air for longer times and can contribute to the transmission of potential viral loads.

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.