arXiv subjects

Alvaro Marin

Publications and source records attributed to Alvaro Marin.

At least 19 recordsLinked to original sources

arXiv2025

Skin formation in evaporating colloidal droplets

When a droplet containing a concentrated suspension evaporates in a dry environment, a layer often forms at the interface accumulating non-volatile material. Such a "skin layer" experiences strong stresses and eventually turns mechanically unstable at the last stage of evaporation. Predicting the formation of such skin layer or particle shell and its properties is a crucial problem for applications and constitutes a multi-scale problem, from the micro/nanoscopic scale of the particles to the millimetric size of the droplets. Interestingly, its physical description lies at the interface between deterministic macroscopic evaporation models and microscopic stochastic particles interactions and diffusion. In this work we present a general theoretical approach to obtain the time-dependent particle concentration profile in an implicit manner, for the general case of diffusion-limited evaporation of spherical droplets, and more generally to all 1D non linear diffusion-limited cases with particles pressure and mobility terms of rational form. This approach is compared successfully to numerical solutions obtained using a finite element solver in the limit of high P\'eclet numbers, and to 2D Brownian dynamics simulations. Our results show that the concentration profiles and shell formation onset depend nontrivially on the initial packing fraction. By analyzing these profiles, we determine the position where the glassy layer forms, whose formation is expected to play a critical role in shell buckling. This model provides a robust framework for predicting the size and maximum aspect ratio of the resulting clusters.

physics.flu-dyn↗

arXiv2024

Evaporating sessile droplets: solutal Marangoni effects overwhelm thermal Marangoni flow

When an evaporating water droplet is deposited on a thermally conductive substrate, the minimum temperature will be at the apex due to evaporative cooling. Consequently, density and surface tension gradients emerge within the droplet and at the droplet-gas interface, giving rise to competing flows from, respectively, the apex towards the contact line (thermal-buoyancy-driven flow) and the other way around (thermal Marangoni flow). In small droplets with a diameter below the capillary length, the thermal Marangoni effects are expected to dominate over thermal buoyancy ("thermal Rayleigh") effects. However, contrary to these theoretical predictions, our experiments mostly show a dominant circulation from the apex towards the contact line, indicating a prevailing of thermal Rayleigh convection. Furthermore, our experiments often show an unexpected asymmetric flow that persisted for several minutes. We hypothesise that a tiny amount of contaminants, commonly encountered in experiments with water/air interfaces, act as surfactants and counteract the thermal surface tension gradients at the interface and thereby promote the dominance of Rayleigh convection. Our finite element numerical simulations demonstrate that, under our specified experimental conditions, a mere 0.5% reduction in the static surface tension caused by surfactants leads to a reversal in the flow direction, compared to the theoretical prediction without contaminants. Additionally, we investigate the linear stability of the axisymmetric solutions, revealing that the presence of surfactants also affects the axial symmetry of the flow.

physics.flu-dyn↗

arXiv2023

Clogging of non-cohesive suspensions through constrictions using an efficient unresolved CFD-DEM solver

When objects are forced to flow through constrictions their transport can be frustrated temporarily or permanently due to the formation of arches in the region of the bottleneck. While such systems have been intensively studied in the case of solid particles in a gas phase being forced by gravitational forces, the case of solid particles suspended in a liquid phase, forced by the liquid itself, has received much less attention. In this case, the influence of the liquid flow on the transport efficiency is not well understood yet, leading to several apparently trivial, but yet unanswered questions, e.g., would an increase of the liquid flow improve the transport of particles or worsen it? Although some experimental data is already available, it lacks enough detail to give a complete answer to such a question. Numerical models would be needed to scrutinize the system deeper. In this paper, we study this system making use of an advanced discrete particle solver (MercuryDPM) and an approximated numerical model for the liquid drag and compare the results with experimental data.

physics.flu-dyn↗

arXiv2022

Interfacial aggregation of self-propelled Janus colloids in sessile droplets

Living microorganisms in confined systems typically experience an affinity to populate boundaries. The reason for such affinity to interfaces can be a combination of their directed motion and hydrodynamic interactions at distances larger than their own size. Here we will show that self-propelled Janus particles (polystyrene particles partially coated with platinum) immersed in droplets of water and hydrogen peroxide tend to accumulate in the vicinity of the liquid/gas interface. Interestingly, the interfacial accumulation occurs despite the presence of an evaporation-driven flow caused by a solutal Marangoni flow, which typically tends to redistribute the particles within the droplet's bulk. By performing additional experiments with passive colloids (flow tracers) and comparing with numerical simulations for both particle active motion and the fluid flow, we disentangle the dominating mechanisms behind the observed interfacial particle accumulation. These results allow us to make an analogy between active Janus particles and some biological microswimmers concerning how they interact with their environment.

physics.flu-dyn↗

arXiv2022

Evaporation-driven liquid flow in sessile droplets

The evaporation of a sessile droplet spontaneously induces an internal capillary liquid flow. The surface-tension driven minimisation of surface area and/or surface-tension differences at the liquid-gas interface caused by evaporation-induced temperature or chemical gradients set the liquid into motion. This flow drags along suspended material and is one of the keys to control the material deposition in the stain that is left behind by a drying droplet. Applications of this principle range from the control of stain formation in the printing and coating industry, to the analysis of DNA, to forensic and medical research on blood stains, and to the use of evaporation-driven self-assembly for nanotechnology. Therefore, the evaporation of sessile droplets attracts an enormous interest from not only the fluid dynamics, but also the soft matter, chemistry, biology, engineering, nanotechnology and mathematics communities. As a consequence of this broad interest, knowledge on evaporation-driven flows in drying droplets has remained scattered among the different fields, leading to various misconceptions and misinterpretations. In this review we aim to unify these views, and reflect on the current understanding of evaporation-driven liquid flows in sessile droplets in the light of the most recent experimental and theoretical advances. In addition, we outline open questions and indicate promising directions for future research.

physics.flu-dyn↗

arXiv2022

Evaporation of a sessile colloidal water-glycerol droplet: Marangoni ring formation

The transport and aggregation of particles in suspensions is an important process in many physicochemical and industrial processes. In this work, we study the transport of particles in an evaporating binary droplet. Surprisingly, the accumulation of particles occurs not only at the contact line (due to the coffee-stain effect) or at the solid substrate (due to sedimentation), but also at a particular radial position near the liquid-air interface, forming a "ring", which we term as the Marangoni ring. The formation of this ring is primarily attributed to the solutal Marangoni flow triggered by the evaporation dynamics of the water-glycerol droplet. Experiments and simulations show fair agreement in the volume evolution and the general structure of the solutal Marangoni flow, that is, the Marangoni vortex. Experiments show that the location of the Marangoni ring is strongly correlated with the Marangoni vortex. However, finite element numerical simulations fail to describe the particle distribution seen in the experiments. Interestingly, the particles not only accumulate to form the Marangoni ring but also assemble as colloidal crystals close to the liquid-air interface, yielding iridescence. The formation of the colloidal crystals in the experiments is strong evidence that non-hydrodynamic interactions, which are not represented in the simulations, also play a significant role in our system.

physics.flu-dyn↗

arXiv2022

Role of liquid driving on the clogging of constricted particle suspensions

Forcing dense suspensions of non-cohesive particles through constrictions might either result in a continuous flow, an intermittent one, or indefinite interruption of flow, i.e., a clog. While one of the most important (and obvious) controlling parameters in such a system is the neck-to-particle size ratio, the role of the liquid driving method is not so obvious. On the one hand, wide-spread volume-controlled systems result in pressure and local liquid velocity increases upon eventual clogs. On the other hand, pressure-controlled systems result in a decrease of the flow through the constriction when a clog is developed. The root of the question therefore lies on the role of interparticle liquid flow and hydrodynamic forces on both the formation and stability of an arch blocking the particle transport through a constriction. In this work, we experimentally analyse a suspension of non-cohesive particles in channels undergoing intermittent regimes, in which they are most sensitive to parametric changes. By exploring the statistical distribution of arrest times and of discharged particles, we surprisingly find that the transport of non-cohesive suspensions through constrictions actually follows a "slower is faster" principle under certain conditions.

physics.flu-dyn↗

arXiv2022

Steering self-organisation through confinement

Self-organisation is the spontaneous emergence of spatio-temporal structures and patterns from the interaction of smaller individual units. Examples are found across many scales in very different systems and scientific disciplines, from physics, materials science and robotics to biology, geophysics and astronomy. Recent research has highlighted how self-organisation can be both mediated and controlled by confinement. Confinement occurs through interactions with boundaries, and can function as either a catalyst or inhibitor of self-organisation. It can then become a means to actively steer the emergence or suppression of collective phenomena in space and time. Here, to provide a common framework for future research, we examine the role of confinement in self-organisation and identify overarching scientific challenges across disciplines that need to be addressed to harness its full scientific and technological potential. This framework will not only accelerate the generation of a common deeper understanding of self-organisation but also trigger the development of innovative strategies to steer it through confinement, with impact, e.g., on the design of smarter materials, tissue engineering for biomedicine and crowd management.

nlin.AO↗

arXiv2021

Influence of Added Dye on Marangoni-driven Droplet Instability

Multiphase flows are challenging systems to study, not only from a fundamental point of view, but also from a practical one due to the difficulties in visualizing phases with similar refraction indices. An additional challenge arises when the multiphase flow to be observed occurs in the sub-millimetric range. A common solution in experimental fluid dynamics is the addition of a color dye for contrast enhancement. However, added dyes can act as surface-active agents and significantly influence the observed phenomena. In the recently reported Marangoni bursting phenomenon, where a binary droplet on top of an oil bath is atomized in thousands of smaller droplets by Marangoni stresses, visualization is particularly challenging and the use of color dyes is naturally tempting. In this work, we quantify experimentally the significant influence of added methyl blue dye, as well as the obtained contrast enhancement. We find that the reaction of the system to such an additive is far from trivial and brings an opportunity to learn about such a complex phenomenon. Additionally, we propose a simple method to analyze the contrast enhancement as a function of dye concentration, with the aim of finding the minimum concentration of dye for successful imaging in similar systems.

physics.flu-dyn↗

arXiv2021

Stability of Respiratory-Like Droplets under Evaporation

Pathogens contained in airborne respiratory droplets have been seen to remain infectious for periods of time that depend on the ambient temperature and humidity. In particular, regarding the humidity, the empirically least favorable conditions for the survival of viral pathogens are found at intermediate humidities. However, the precise physico-chemical mechanisms that generate such least-favorable conditions are not understood yet. In this work, we analyze the evaporation dynamics of respiratory-like droplets in air, semi-levitating them on superhydrophobic substrates with minimal solid-liquid contact area. Our results reveal that, compared to pure water droplets, the salt dissolved in the droplets can significantly change the evaporation behaviour, especially for high humidities close to and above the deliquesence limit. Due to the hygroscopic properties of salt, water evaporation is inhibited once the salt concentration reaches a critical value that depends on the relative humidity. The salt concentration in a stable droplet reaches its maximum at around 75% relative humidity, generating conditions that might shorten the time in which pathogens remain infectious.

physics.flu-dyn↗

arXiv2020

Catastrophic phase inversion in high-Reynolds number turbulent Taylor--Couette flow

Emulsions are omnipresent in the food industry, health care, and chemical synthesis. In this Letter the dynamics of meta-stable oil-water emulsions in highly turbulent ($10^{11}\leq\text{Ta}\leq 3\times 10^{13}$) Taylor--Couette flow, far from equilibrium, is investigated. By varying the oil-in-water void fraction, catastrophic phase inversion between oil-in-water and water-in-oil emulsions can be triggered, changing the morphology, including droplet sizes, and rheological properties of the mixture, dramatically. The manifestation of these different states is exemplified by combining global torque measurements and local in-situ laser induced fluorescence (LIF) microscopy imaging. Despite the turbulent state of the flow and the dynamic equilibrium of the oil-water mixture, the global torque response of the system is found to be as if the fluid were Newtonian, and the effective viscosity of the mixture was found to be several times bigger or smaller than either of its constituents.

physics.flu-dyn↗

arXiv2020

Dissolution of microdroplets in a sparsely miscible liquid confined by leaky walls

When a water droplet is deposited within a sparsely miscible liquid medium such as certain oils, the droplet surprisingly vanishes, even in a confined geometry. Such a phenomenon has crucial consequences for multiphase flows in which confined nano- and/or picoliter droplets are considered. We report here experiments of microdroplet dissolution in microchannels that reveal an enhancement of the shrinkage of confined water microdroplets in oil due to the permeability of the walls - made of polydimethilsiloxane (PDMS) - and a delay when collective effects are present. The system is first modelled assuming that the dissolution of the droplets in its surrounding liquid follows the Epstein-Plesset solution of the diffusion equation. The dissolution of small isolated droplets can indeed be described by this solution of the diffusion equation, while the vanishing of droplets larger than a certain critical value and those closer to other droplets requires numerical simulations which take into account the boundary conditions of the confined system, the neighbouring droplets and interestingly, the evaporative water vapour flux through the PDMS. Our results thus reveal the important role of the water solubility in oil and most remarkably, of the water vapour transport through permeable walls.

physics.flu-dyn↗

arXiv2020

Size-dependent particle migration and trapping in 3D microbubble streaming flows

Acoustically actuated sessile bubbles can be used as a tool to manipulate microparticles, vesicles and cells. In this work, using acoustically actuated sessile semi-cylindrical microbubbles, we demonstrate experimentally that finite-sized microparticles undergo size-sensitive migration and trapping towards specific spatial positions in three dimensions with high reproducibility. The particle trajectories are successfully reproduced by passive advection of the particles in a steady three-dimensional streaming flow field augmented with volume exclusion from the confining boundaries. For different particle sizes, this volume exclusion mechanism leads to three regimes of qualitatively different migratory behavior, suggesting applications for separating, trapping, and sorting of particles in three dimensions.

physics.flu-dyn↗

arXiv2020

Transition from clogging to continuous flow in constricted particle suspensions

When suspended particles are pushed by liquid flow through a constricted channel they might either pass the bottleneck without trouble or encounter a permanent clog that will stop them forever. However, they may also flow intermittently with great sensitivity to the neck-to-particle size ratio D/d. In this work, we experimentally explore the limits of the intermittent regime for a dense suspension through a single bottleneck as a function of this parameter. To this end, we make use of high time- and space-resolution experiments to obtain the distributions of arrest times T between successive bursts, which display power-law tails with characteristic exponents. These exponents compare well with the ones found for as disparate situations as the evacuation of pedestrians from a room, the entry of a flock of sheep into a shed or the discharge of particles from a silo. Nevertheless, the intrinsic properties of our system i.e. channel geometry, driving and interaction forces, particle size distribution seem to introduce a sharp transition from a clogged state to a continuous flow, where clogs do not develop at all. This contrasts with the results obtained in other systems where intermittent flow, with power-law exponents above two, were obtained.

physics.flu-dyn↗

arXiv2019

Pattern formation by droplet evaporation and imbibition in watercolor paintings

Watercolor or aquarelle is one of the oldest painting methods in which pigments suspended in an aqueous liquid are deposited over a substrate, typically an absorbing material such as paper. The physical processes which lead to pattern formation have not been studied in any depth, in spite of being closely related to flows in other contexts. Identifying and understanding these processes is of imperative importance to restore and preserve watercolor paintings. Here, we report an experimental study of the effect of the pigment concentration and paper humidity on the pattern formation derived from evaporation of droplets of watercolor paintings. Optical analysis reveals the formation of color gradients, stratifications, flat regions, borders, dendritic shapes, and radial tips. We found that droplet evaporation on dry paper forms ring-shaped stains which resemble to the \emph{coffee-stain effect} regardless of the nature of the pigment. The mean pixel intensity of such deposits follows an exponential function that saturates at high concentration, while the thickness of the coffee ring increase for watercolor inks containing colloidal particles and does not change for non-colloidal . Our experiments reveal that water distribution on the paper surface, and not the volumetric absorption of water on the paper, determine the structural characteristics of watercolor stains. We show evidence that the cornerstone in the creation of complex patterns in watercolor paintings is driven by the coffee ring effect and imbibition processes. Our findings aim to serve as framework for further investigations of the complex processes involved in this ancient art form and could guide restoration processes needed to preserve the heritage value of historical watercolor artworks.

physics.flu-dyn↗

arXiv2019

Bacterial Footprints in Elastic Pillared Microstructures

Soft substrates decorated with micropillar arrays are known to be sensitive to deflection due to capillary action. In this work, we demonstrate micropillared epoxy surfaces are sensitive to single drops of bacterial suspensions. The micropillars can show significant deformations upon evaporation, just as capillary action does in soft substrates. The phenomenon has been studied with five bacterial strains S. epidermidis, L. sakei, P. aeruginosa, E. coli and B. subtilis. The results reveal that only droplets containing motile microbes with flagella stimulate micropillar bending, which leads to significant distortions and pillar aggregations forming dimers, trimers, and higher order clusters. Such deformation is manifested in characteristic patterns that are left on the microarrayed surface following evaporation, and can be easily identified even by the naked eye. Our findings could lay the ground for the design and fabrication of mechanically responsive substrates, sensitive to specific types of microorganisms.

cond-mat.soft↗

arXiv2019

Interfacial flows in sessile evaporating droplets of mineral water

Liquid flow in sessile evaporating droplets of ultrapure water typically results from two main contributions: a capillary flow pushing the liquid towards the contact line from the bulk and a thermal Marangoni flow pulling the drop free surface towards the summit. Current analytical and numerical models are in good qualitative agreement with experimental observations however they overestimate the interfacial velocity values by 2-3 orders of magnitude. This discrepancy is generally ascribed to contamination of the water samples with non-soluble surfactants, however an experimental confirmation of this assumption has not yet been provided. In this work, we show that a small "ionic contamination" can cause a significant effect in the flow pattern inside the droplet. To provide the proof, we compare the flow in evaporating droplets of ultrapure water with commercially available bottled water of different mineralization levels. Mineral waters are bottled at natural springs, are micro-biologically pure, and contain only traces of minerals (as well as traces of other possible contaminants), therefore one would expect a slower interfacial flow as the amount of "contaminants" increase. Surprisingly, our results show that the magnitude of the interfacial flow is practically the same for mineral waters with low content of minerals as that of ultrapure water. However, for waters with larger content of minerals, the interfacial flow tends to slow down due to the presence of ionic concentration gradients. Our results show a much more complex scenario than it has been typically suspected, and therefore a deeper and more comprehensive analysis of the huge differences between numerical models and experiments is necessary.

physics.flu-dyn↗

arXiv2018

Solutal Marangoni flow as the cause of ring stains from drying salty colloidal drops

Evaporating salty droplets are ubiquitous in nature, in our home and in the laboratory. Interestingly, the transport processes in such apparently simple systems differ strongly from evaporating "freshwater" droplets since convection is partly inverted due to Marangoni stresses. Such an effect has crucial consequences to the salt crystallization process and to the deposits left behind. In this work we show unprecedented measurements that, not only confirm clearly the patterns of the flow inversion, but also elucidate their impact on the distribution of non-volatile solutes. Contrary to what has been often reported in the literature, such a flow reversal does not prevent the formation of ring-shaped stains: particles accumulate at the contact line driven solely by the interfacial flow. We can therefore conclude that the classical "coffee-stain effect" is not the only mechanism that can generate ring-shaped stains in evaporating droplets.

physics.flu-dyn↗