Surveying the Directional Transport of Water Droplets upon Impact on Metallic Topographic Gradients.

Drop impact phenomena on raw, polished, and topography-altered gradient surfaces are investigated and presented. The main aim of this study is to demonstrate that in using a one-step industrial patterning process, it is possible to obtain metal topographical wetting gradients that can produce various desired outcomes after droplet impact. The findings could be applied to improving wind or steam turbine blades. The ranges of Weber (We) and Reynolds (Re) numbers in the study are 3-300 and 650-6500, respectively. It is demonstrated that for a fixed We, the droplet transport outcomes change from bouncing-off to side-flipping to deposition depending on the impact location and the gradient strength. The effect of We in combination with the gradient strength was also considered to demonstrate droplet behavior similar to that observed on a uniform water repellent surface and on biphilic systems. In addition, full bouncing-off and directional control have been demonstrated. For the condition We = 95 ± 3, it was possible to achieve a maximum droplet recoil height of ∼6 mm and a side motion of almost 8 mm. A combination of different outcomes (e.g., splashing on one side of a droplet and passive horizontal translation on another) was observed on the studied gradients at We > 200 due to different wetting regimes across the droplet's three-phase line.

Influence of rheology and micropatterns on spreading, retraction and fingering of an impacting drop.

Rheology and surface microstructure affect many drop impact processes, including in emerging printing and patterning applications. This study reports on experiments systematically addressing the influence of these parameters on drop impacts. The experiments involved drop impacts of water, glycerol, and shear-thinning carbopol solutions on ten different microstructured surfaces, captured using high-speed photography. The impact Weber number (We) was varied from 70 to 350, and the microstructures consisted of 20 µm wide pillars with circular and square cross sections arranged in square arrays. The data focus on maximum spreading, retraction rates, threshold conditions for asymmetric (non-circular) spreading, and fingers protruding from the spreading rim. The extent of spreading was reduced by the presence of micropillars, and was well-explained using a hybrid scaling model. The drop retraction rate () showed moderate agreement with the inertial regime scaling  ∝ We-0.50, but did decrease with effective viscosity. Retraction was slower when the contact line was pinned on surfaces that were flat or had relatively tall or closely-spaced pillars, and was disrupted by drop break-up at We ≳ 250 for low-viscosity fluids. Impact velocities at the onset of asymmetric spreading had weak dependence on viscosity. Fingers were more numerous for greater We, lower effective viscosity, lower pillar height, and for pillars with square cross-sections. Fingers were favoured in directions parallel to the rows of the pillar array, especially near the onset of finger formation. Consistent comparisons between Newtonian and non-Newtonian fluids were enabled by calculating an effective Reynolds number.

Ferrofluid drop impacts and Rosensweig peak formation in a non-uniform magnetic field.

Vertical drop impacts of ferrofluids onto glass slides in a non-uniform magnetic field have been studied using high-speed photography. Outcomes have been classified based on the motion of the fluid-surface contact lines, and formation of peaks (Rosensweig instabilities) which affect the height of the spreading drop. The largest peaks are nucleated at the edge of a spreading drop, similarly to crown-rim instabilities in drop impacts with conventional fluids, and remain there for an extended time. Impact Weber numbers ranged from 18.0 to 489, and the vertical component of the B-field was varied between 0 and 0.37 T at the surface by changing the vertical position of a simple disc magnet placed below the surface. The falling drop was aligned with the vertical cylindrical axis of the 25 mm diameter magnet, and the impacts produced Rosensweig instabilities without splashing. At high magnetic flux densities a stationary ring of ferrofluid forms approximately above the outer edge of the magnet.

Biomechanical responses of encysted zoospores of the oomycete Achlya bisexualis to hyperosmotic stress are consistent with an ability to turgor regulate.

Zoospores are motile, asexual reproductive propagules that enable oomycete pathogens to locate and infect new host tissue. While motile, they have no cell wall and maintain tonicity with their external media using water expulsion vacuoles. Once they locate host tissue, they encyst and form a cell wall, enabling the generation of turgor pressure that will provide the driving force for germination and invasion of the host. It is not currently known how these spores respond to the osmotic stresses that might arise due to different environments on and around their hosts that have different osmotic strengths. We have made microaspiration (MA) measurements on > 800 encysted zoospores and atomic force microscopy (AFM) measurements on 12 encysted zoospores to determine their mechanical properties and how these change after hyperosmotic stress. Two types of encysted zoospores (Type A and Type B) were produced from the oomycete Achlya bisexualis, that differed in their morphology and response. With a small hyperosmotic stress (using 0.1 and 0.2 M sorbitol to give media osmolality changes of 155.4 and 295.6 mOsmol/kg), Type A zoospores initially became stiffer, with an increase in the Young's modulus (E) over 30 mins from 0.16 MPa to 0.25 and 0.22 MPa respectively. E then returned to its original value after 120 min. With a greater osmotic stress (using 0.3, 0.4 and 0.5 M sorbitol to give media osmolality changes of 438.2, 587.2 and 787.6 mOsmol/kg) the reverse occurred, with an initial decrease in E over 30 - 60 mins to values of 0.1, 0.08 and 0.09 MPa respectively, before recovery to the original value after 120 min. In 0.5 M sorbitol this recovery was only observed with AFM, but not with MA. Type B zoospores, which may be primary/secondary spores about to release secondary/tertiary spores, or else spores that were damaged during encystment, initially stiffened in response to the lower hyperosmotic stresses with a slight increase in E (from 0.077 to 0.1 MPa after 15 min (with both 0.1 and 0.2 M sorbitol) before recovering to the original value after 60 min. These spores showed no change in response to the higher osmotic stresses. The responses of the Type A spores are consistent with rapid changes in cell wall thickness and a turgor regulation mechanism. Turgor regulation is further supported by microscopic observations of the Type A spores showing protoplast retraction from the cell wall followed by deplasmolysis, coupled with measurements of spore volume. As far as we are aware this is the first demonstration of turgor regulation, not just in encysted zoospores, but in oomycetes in general.

Asymmetric assembly of Lennard-Jones Janus dimers.

Self-assembly of Janus (or "patchy") particles is dependent on the precise interaction between neighboring particles. Here, the orientations of two amphiphilic Janus spheres within a dimer in an explicit fluid are studied with high geometric resolution. Molecular dynamics simulations and semianalytical energy calculations are used with hard- and soft-sphere Lennard-Jones potentials, and temperature and hydrophobicity are varied. The most probable center-center-pole angles are in the range of 40^{∘}-55^{∘} with pole-to-pole alignment not observed due to orientational entropy. Angles near 90^{∘} are energetically unfavored due to solvent exclusion, and the relative azimuthal angle between the spheres is affected by solvent ordering. Relatively large polar angles become more favored as the hydrophobic surface area (i.e., Janus balance) is increased.

Depletion of HP1α alters the mechanical properties of MCF7 nuclei.

Within the nucleus of the eukaryotic cell, DNA is partitioned into domains of highly condensed, transcriptionally silent heterochromatin and less condensed, transcriptionally active euchromatin. Heterochromatin protein 1α (HP1α) is an architectural protein that establishes and maintains heterochromatin, ensuring genome fidelity and nuclear integrity. Although the mechanical effects of changes in the relative amount of euchromatin and heterochromatin brought about by inhibiting chromatin-modifying enzymes have been studied previously, here we measure how the material properties of the nuclei are modified after the knockdown of HP1α. These studies were inspired by the observation that poorly invasive MCF7 breast cancer cells become more invasive after knockdown of HP1α expression and that, indeed, in many solid tumors the loss of HP1α correlates with the onset of tumor cell invasion. Atomic force microscopy (AFM), optical tweezers (OT), and techniques based on micropipette aspiration (MA) were each used to characterize the mechanical properties of nuclei extracted from HP1α knockdown or matched control MCF7 cells. Using AFM or OT to locally indent nuclei, those extracted from MCF7 HP1α knockdown cells were found to have apparent Young's moduli that were significantly lower than nuclei from MCF7 control cells, consistent with previous studies that assert heterochromatin plays a major role in governing the mechanical response in such experiments. In contrast, results from pipette-based techniques in the spirit of MA, in which the whole nuclei were deformed and aspirated into a conical pipette, showed considerably less variation between HP1α knockdown and control, consistent with previous studies reporting that it is predominantly the lamins in the nuclear envelope that determine the mechanical response to large whole-cell deformations. The differences in chromatin organization observed by various microscopy techniques between the MCF7 control and HP1α knockdown nuclei correlate well with the results of our measured mechanical responses and our hypotheses regarding their origin.

Stability of amphiphilic Janus dimers in shear flow: a molecular dynamics study.

Amphiphilic Janus particles in a flow are thought to experience a torque due to the asymmetry in slip at their surfaces. This effect has the potential to destabilise self-assembled Janus structures in flows due to the forces and torques applied to individual Janus nanoparticles. In this work, we investigate the stability of amphiphilic Janus dimers and homogeneous hydrophobic dimers in shear flow using molecular dynamics, and study possible break-up mechanisms. In particular, we consider the influence of the activation enthalpy and entropy on the thermal break-up rate of these dimers. Janus dimers are less stable than hydrophobic dimers, and increasing the applied shear rate has a greater effect on break-up for Janus dimers. Two mechanisms leading to increased break-up in shear flow are studied, namely the rotational speed of the dimers and the orientation of individual spheres in the dimers, and we propose a descriptive equation for calculation of the break-up rate. Overall, the results indicate that the stability of dimers in shear flow depends on the slip length at the spheres' surfaces, and that the slip length difference on Janus dimers could contribute to destabilisation.

Inertial capillary uptake of drops.

Uptake of liquid drops into capillary tubes has been experimentally studied and quantitatively analyzed. In experiments, drops of water and aqueous glycerol (≤50 wt %) were drawn into cylindrical borosilicate glass and quartz tubes with an inner diameter of 0.50-0.75 mm. The meniscus height rise was measured using high-speed images captured at 4000 frames per second, and results within a conservatively defined inertial regime indicate constant uptake velocity. An increase in the inertial velocity with drop curvature was observed due to increasing Laplace pressure in the drop, as drop sizes were comparable to the width of the capillary tubes. Measured velocities were slower than predicted by a purely inertial-capillary model and best described by introducing a contact line friction, consistent with the observed variability and viscosity dependence of the results. Mean friction coefficients in borosilicate capillaries ranged from 169±1 for 50 wt % glycerol drops to 218±1 for water drops. Peaks in the instantaneous Laplace pressure caused by surface oscillations were also measured. Correlations with uptake velocity were qualitatively apparent, with a delay between peaks of similar magnitude to the inertial-capillary oscillation time.

High Throughput Analysis of Liquid Droplet Impacts.

Experimental studies of liquid drop impacts on surfaces are often restricted in their scope due to the large range of possible experimental parameters such as material properties, impact conditions, and experimental configurations. Compounding this, drop impacts are often studied using data-rich high-speed photography, so that it is difficult to analyze many experiments in a detailed and timely manner. The purpose of this method is to enable efficient study of droplet impacts with high-speed photography by using a systematic approach. Equipment is aligned and calibrated to produce videos that can be accurately processed by a custom image processing code. Moreover, the file structure setup and workflow described here ensure efficiency and clear organization of data processing, which is carried out while the researcher is still in the lab. The image processing method extracts the digitized outline of the impacting droplet in each frame of the video, and processed data are stored for further analysis as required. The protocol assumes that a droplet is released vertically under gravity, and impact is recorded by a camera viewing from side-on with the drop illuminated using shadowgraphy. Many similar experiments involving image analysis of high-speed events could be addressed with minor adjustment to the protocol and equipment used.

Use of microaspiration to study the mechanical properties of polymer gel microparticles.

The mechanical properties of polyacrylamide (PA) and polydimethylsiloxane (PDMS) microparticle populations have been measured using microaspiration, a recently developed experimental technique. Microaspiration is an augmented version of micropipette aspiration, in which optical microscopy data are obtained as individual soft particles pass through the tip of a micropipette. During microaspiration, the ion current passing through the pipette tip is also measured, and the synchronised optical and current data streams are used to study and quantify mechanical properties. Ion current signatures for the poroelastic PA particles were qualitatively different from those of the viscoelastic PDMS particles. For PA particles the current gradually reduced during each aspiration event, whereas for PDMS particles the current trace resembled a negative top hat function. For PA particles it was found that the maximum change in current during aspiration (ΔIh) increased with particle size. By considering the initial elastic response, a mean effective shear modulus (G') of 6.6 ± 0.2 kPa was found for aspiration of 115 PA particles of ∼10-20 µm diameter. Using a viscoelastic model to describe flow into the pipette, a mean initial effective elastic modulus (E0') of 3.5 ± 1.7 MPa was found for aspiration of 17 PDMS particles of ∼ 9-11 µm diameter. These moduli are consistent with previously reported literature values, providing initial validation of the microaspiration method.

Molecular dynamics simulations of Janus nanoparticles in a fluid flow.

We study the forces and torques on individual Janus nanoparticles in a fluid flow using molecular dynamics simulations. In particular, we consider amphiphilic Janus nanospheres that have different slip boundary conditions on each hemisphere, and calculate the forces and torques experienced by them as a function of their orientation with respect to the flow direction. Furthermore, we examine nanoparticles that are deformed slightly from a spherical shape, and have no-slip boundary conditions. We compare the simulation results to the predictions of previously introduced theoretical approaches, which compute the forces and torques on particles with variable slip lengths or aspherical deformations that are much smaller than the particle radius. We found that there is good qualitative agreement between the forces and torques computed from our simulations and the theoretical predictions, and the forces quantitatively agree when the assumptions made in the theoretical descriptions are satisfied.

Mechanical properties of bovine erythrocytes derived from ion current measurements using micropipettes.

Synchronized data from ion currents and optical microscopy have been used to measure the mechanical properties of individual soft microparticles. This new experimental method draws on the signals generated by each particle as it passes through the tip of a pipette. The technique represents an advance on micropipette aspiration (MA), which uses optical microscopy in isolation. The ionic resistance through the tip provides additional information regarding the progress of particle deformation. The augmented technique is demonstrated by studying aspiration of individual bovine erythrocytes into a micropipette. Effective mechanical properties have been deduced by using the ionic current response to measure the dwell time and velocity of erythrocytes. Values obtained for the effective viscosity represent liquid-like deformation of the whole cell, and show a consistent shear thinning effect. The effective elasticity also varies with applied force, and was higher for erythrocytes stored for several weeks. The data show that wall friction is an important factor for the uptake dynamics, and that the erythrocytes were damaged or ruptured when passing through pipettes of opening diameter 0.7 µm, the smallest used. These results demonstrate a new approach to measuring the mechanics of individual bioparticles.

Preclinical studies evaluating the effect of semifluorinated alkanes on ocular surface and tear fluid dynamics.

PURPOSE: Dry eye disease (DED) is one of the most prevalent ocular surface disorders that presents clinically. Recently, the semifluorinated alkane (SFA) perfluorohexyloctane (NovaTears®; EvoTears®) entered the market for the management of evaporative DED, while perfluorobutylpentane has been used as a vehicle to enhance ocular drug delivery. This study evaluated the mechanisms by which SFAs might improve therapeutic outcomes in DED. METHODS: Interactions of both SFAs with the corneal surface were evaluated ex vivo using high-speed photography. The in vivo influence of SFAs on tear fluid dynamics was evaluated in healthy rabbit eyes observing changes in lipid layer grade, tear evaporation rate, tear volume and tear osmolarity. Furthermore, ocular tolerability was confirmed by clinical scoring and sodium fluorescein staining. RESULTS: Ex vivo studies demonstrated that both SFAs rapidly spread on the ocular surface with their contact angle on the cornea being virtually zero. A significant improvement in lipid layer grade was observed immediately after instillation of both SFAs in vivo, although the improvement was more sustained upon instillation of perfluorohexyloctane with a statistically significant difference compared to saline instillation evident from day five onwards. No significant changes in tear evaporation rate, volume or osmolarity, nor any signs of ocular irritation were observed after application of either SFA over the seven-day study period. CONCLUSION: Both SFAs showed excellent spreading on the ocular surface. Perfluorohexyloctane improved the lipid layer grade significantly after topical application supporting its potential to stabilise the tear film lipid layer and thus provide symptomatic relief in evaporative DED.

Tunable Resistive Pulse Sensing: Better Size and Charge Measurements for Submicrometer Colloids.

Tunable resistive pulse sensing (TRPS) uses the Coulter principle to detect, measure, and analyze particles at length scales ranging from tens of nanometers through to micrometers. The technology and its associated methods have advanced so that TRPS is regularly used as a characterization technique in peer-reviewed studies. This Perspective is concerned with opportunities to further develop TRPS, with a specific focus on improved measurement of size and charge for submicrometer particles. There is currently broad demand for increased rigor in such measurements. Particular points of interest include consistent use of statistics, development of accurate physical models, and realistic assessment of uncertainties associated with the usual measurement protocols. Highlights from recent studies involving TRPS are also reviewed. The technique is particularly popular in the burgeoning research field relating to extracellular vesicles, and the range of biologically relevant applications also includes liposomes, viruses, and on-bead assays.

Scanning ion conductance microscopy mapping of tunable nanopore membranes.

We report on the use of scanning ion conductance microscopy (SICM) for in-situ topographical mapping of single tunable nanopores, which are used for tunable resistive pulse sensing. A customised SICM system was used to map the elastomeric pore membranes repeatedly, using pipettes with tip opening diameters of approximately 50 nm and 1000 nm. The effect of variations on current threshold, scanning step size, and stretching has been studied. Lowering the current threshold increased the sensitivity of the pipette while scanning, up to the point where the tip contacted the surface. An increase in the pore area was observed as the step size was decreased, and with increased stretching. SICM reveals details of the electric field near the pore entrance, which is important for understanding measurements of submicron particles using resistive pulse sensing.

Pulse Size Distributions in Tunable Resistive Pulse Sensing.

The use of resistive pulse sensors for submicron particle size measurements relies on a clear understanding of pulse size distributions. Here, broadening of such distributions has been studied and explained using conical pores and nominally monodisperse polystyrene particles 200-800 nm in diameter. The use of tunable resistive pulse sensing (TRPS) enabled continuous in situ control of the pore size during experiments. Pulse size distributions became broader when the pore size was increased and featured two distinct peaks. Similar distributions were generated using finite element simulations, which suggested that relatively large pulses are produced by particles with trajectories passing near to the edge of the pore. Other experiments determined that pulse size distributions are independent of applied voltage but broaden with increasing pressure applied across the membrane. The applied pressure could also be reversed in response to a pulse, which enabled repeated measurement of individual particles moving back and forth through the pore. Hydrodynamic and electrophoretic focusing each appear to affect particle trajectories under certain conditions.

Asymmetries in the spread of drops impacting on hydrophobic micropillar arrays.

Studies of water drop impacts on microstructured surfaces are important for understanding dynamic wetting on rough surfaces, and for developing related design principles. Here, high-speed imaging has been used to study asymmetries within the spreading phase following vertical water drop impacts at Weber numbers between 34 and 167. The eleven polydimethylsiloxane surfaces studied had micropillars arranged in square and rectangular arrays, with feature sizes ranging from ∼5 µm to ∼240 µm and various pillar cross-sections, in most cases supporting a static Cassie state. Two contrasting and apparently independent asymmetries were identified. Firstly, partial (rather than full) microstructure penetration occurred on five of the surfaces, with the edges of the penetrated profiles tending to lie parallel to the array rows and columns. These observations are best explained by considering surface energies. Secondly, the perimeter of a spreading drop tends to lie at 45° to the rows and columns. This shape is caused by movement of air from underneath the impacting drop, which generates jets and subsequent fingers in preferred directions at the edge of the drop. The area of the 'corridor' through which the air escapes is an important quantitative parameter. Experiments also demonstrate the effects of microstructures on the maximum spreading diameter, and formation of off-centre microbubble patterns.

Conductive and biphasic pulses in tunable resistive pulse sensing.

This experimental study concerns the occurrence of biphasic pulses generated during tunable resistive pulse sensing (TRPS) of 200 nm carboxylate polystyrene spheres. In TRPS, a short-lived pulse in ionic current is observed when an individual colloid passes through a pore which separates two fluid reservoirs. The pulse is conventionally resistive, but conductive pulses are observed under certain experimental conditions, as well as biphasic pulses which include both resistive and conductive components. The experimental variables investigated here include the concentration of the phosphate-buffered saline electrolyte, particle charge, pore size, applied voltage, and the direction of particle motion. The onset upper electrolyte concentration for biphasic pulses in TRPS is ∼50 mM, and the ordering of biphasic pulse components can be interpreted using ionic concentration polarization if the conductive component is generated when the particle is in the ion depletion region. Besides providing fundamental understanding, the results are important for the TRPS technique, which is becoming widely used for particle-by-particle measurements of submicron colloids.

Applications of tunable resistive pulse sensing.

Tunable resistive pulse sensing (TRPS) is an experimental technique that has been used to study and characterise colloidal particles ranging from approximately 50 nm in diameter up to the size of cells. The primary aim of this Review is to provide a guide to the characteristics and roles of TRPS in recent applied research. Relevant studies reflect both the maturation of the technique and the growing importance of submicron colloids in fields such as nanomedicine and biotechnology. TRPS analysis of extracellular vesicles is expanding particularly swiftly, while TRPS studies also extend to on-bead assays using DNA and aptamers, drug delivery particles, viruses and bacteria, food and beverages, and superparamagnetic beads. General protocols for TRPS measurement of particle size, concentration and charge have been developed, and a summary of TRPS technology and associated analysis techniques is included in this Review.

Co-ordinated detection of microparticles using tunable resistive pulse sensing and fluorescence spectroscopy.

Tunable resistive pulse sensing (TRPS) has emerged as a useful tool for particle-by-particle detection and analysis of microparticles and nanoparticles as they pass through a pore in a thin stretchable membrane. We have adapted a TRPS device in order to conduct simultaneous optical measurements of particles passing through the pore. High-resolution fluorescence emission spectra have been recorded for individual 1.9 µm diameter particles at a sampling period of 4.3 ms. These spectra are time-correlated with RPS pulses in a current trace sampled every 20 µs. The flow rate through the pore, controlled by altering the hydrostatic pressure, determines the rate of particle detection. At pressures below 1 kPa, more than 90% of fluorescence and RPS events were matching. At higher pressures, some peaks were missed by the fluorescence technique due to the difference in sampling rates. This technique enhances the particle-by-particle specificity of conventional RPS measurements and could be useful for a range of particle characterization and bioanalysis applications.