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Howard A. Stone

Publications and source records attributed to Howard A. Stone.

At least 37 records · Page 2Linked to original sources

Design of model Boger fluids with systematically controlled viscoelastic properties

The subject of viscoelastic flow phenomena is crucial to many areas of engineering and the physical sciences. Although much of our understanding of viscoelastic flow features stems from carefully designed experiments, preparation of model viscoelastic fluids remains a challenge; for example, fabricating a series of fluids with different fluid shear moduli $G_0$, but with an identical relaxation time $τ$, is nontrivial. In this work, we harness the non-ideality of nearly constant-viscosity elastic fluids, commonly known as `Boger fluids', made with polyisobutylene, to develop an experimental methodology that produces a set of fluids with desired viscoelastic properties, specifically, $G_0$, $τ$, and the first normal stress difference coefficient $ψ_1$. Through a linear algebraic relation between the rheological properties of interest ($G_0$, $τ$, $ψ_1$) and the fluid compositions in terms of polymer concentration $c$, molecular weight $M_w$, and solvent viscosity $η_s$, we developed a `design equation' that takes $G_0$, $τ$, $ψ_1$ as inputs and calculates values for $c$, $M_w$, $η_s$ as outputs. Using this method, fabrication of dilute viscoelastic fluids whose rheological properties are \textit{a priori} known can be achieved.

cond-mat.soft↗

Retraction Dynamics of a Highly Viscous Liquid Sheet

We study the one-dimensional capillary-driven retraction of a finite, planar liquid sheet in the asymptotic regime where both the Ohnesorge number $\mathrm{Oh}$ and the initial length-to-thickness ratio $l_0/h_0$ are large. In this regime, the fluid domain decomposes into two regions: a thin-film region governed by one-dimensional mass and momentum equations, and a small tip region near the free edge described by a self-similar Stokes flow. Asymptotic matching between these regions yields an effective boundary condition for the thin-film region, representing a balance between viscous and capillary forces at the free edge. Surface tension drives the thin-film flow only through this boundary condition, while the local momentum balance is dominated by viscous and inertial stresses. We show that the thin-film flow possesses a conserved quantity, reducing the equation of thickness to heat equation with time-dependent boundary conditions. The reduced problem depends on a single dimensionless parameter $\mathcal{L} = l_0 / (4 h_0 \mathrm{Oh})$. Numerical solutions of the reduced model agree well with previous studies and reveal that the sheet undergoes distinct retraction regimes depending on $\mathcal{L}$ and a dimensionless time after rupture $T$. We derive asymptotic approximations for the thickness profile, velocity profile, and retraction speed during the early and late stages of retraction. At early times, the retraction speed grows as $T^{1/2}$, while at late times it decays as $1/T^2$. An intermediate regime arises for very long sheets ($\mathcal{L} \gg 1$). During this phase, the retraction speed approaches the Taylor-Culick value. When $T \approx \mathcal{L}$, the speed undergoes fast deceleration from the Taylor-Culick speed to late-time asymptotics.

physics.flu-dyn↗

Flash Freeze--Thaw Phenomenon in Sprayed Evaporating Micrometer Droplets

Two-fluid spray nozzles are widely used in combustion, chemical processing, pharmaceutical coating, environmental control, and spray drying to atomize liquids with pressurized gas. However, the adiabatic cooling and resulting flash freeze--thaw exposure of atomized droplets remain underexplored. Using high-fidelity computational fluid dynamics coupled with droplet-scale nucleation modeling, we show that the atomizing gas temperature at the nozzle exit can fall from $22\,^{\circ}\mathrm{C}$ to below $-130\,^{\circ}\mathrm{C}$, initiating rapid ice nucleation and freezing in micro-scale droplets. For atomizing gas at $5\,\mathrm{bar}$ (gauge) and $22\,^{\circ}\mathrm{C}$, all droplets smaller than $1.5\,μ\mathrm{m}$ freeze, whereas droplets larger than $3\,μ\mathrm{m}$ remain liquid. These frozen droplets thaw within $O(10)\,μ\mathrm{s}$ upon leaving the cold zone, subjecting sensitive actives to intense freeze--thaw thermomechanical stresses near the nozzle even when the bulk drying gas is warm. Parametric studies show that ice formation is eliminated at atomizing gas temperatures above $110\,^{\circ}\mathrm{C}$ for all gas-to-liquid mass ratios (GLRs) between 8 and 25, or at $\mathrm{GLR}<12$ for all atomizing gas temperatures; the chamber drying gas does not influence near-nozzle freezing. Additionally, we demonstrate that swirling flow intensifies flash freeze--thaw by deepening gas cooling, whereas non-swirling flow extends cold-zone residence time, yet both designs produce similar iced-droplet fractions. We construct an operating map delineating conditions that avoid flash freeze--thaw and show that the no-ice boundary provides a conservative criterion for both swirl and non-swirl nozzles. These findings identify a previously unrecognized freeze--thaw stress mechanism that can compromise spray-dried pharmaceutical product stability.

physics.flu-dyn↗

Coalescence of viscoelastic sessile drops: the small and large contact angle limits

The coalescence and breakup of drops are classic examples of flows that feature singularities. The behavior of viscoelastic fluids near these singularities is particularly intriguing - not only because of their added complexity, but also due to the unexpected responses they often exhibit. In particular, experiments have shown that the coalescence of viscoelastic sessile drops can differ significantly from their Newtonian counterparts, sometimes resulting in a sharply defined interface. However, the mechanisms driving these differences in dynamics, as well as the potential influence of the contact angle are not fully known. Here, we study two different flow regimes effectively induced by varying the contact angle and demonstrate how that leads to markedly different coalescence behaviors. We show that the coalescence dynamics is effectively unaltered by viscoelasticity at small contact angles. The Deborah number, which is the ratio of the relaxation time of the polymer to the timescale of the background flow, scales as $θ^3$ for $θ\ll 1$, thus rationalizing the near-Newtonian response. On the other hand, it has been shown previously that viscoelasticity dramatically alters the shape of the interface during coalescence at large contact angles. We study this large contact angle limit using experiments and 2D numerical simulations of the equation of motion. We show that the departure of the coalescence dynamics from the Newtonian case is a function of the Deborah number and the elastocapillary number, which is the ratio between the shear modulus of the polymer solution and the characteristic stress in the fluid.

physics.flu-dyn↗

Soft-Lubrication Drainage and Rupture in Particle-Driven Vesicles

The deformation and rupture of a lipid vesicle due to the forced normal approach of an inclusion are essential for optimizing the design of magnetic giant unilamellar vesicles [magGUVs, Malik et al., Nanoscale 17, 13720 (2025)], with implications for active colloid-membrane interactions and cellular-scale chemical delivery. Here, we investigate vesicles propelled by a force-driven rigid inclusion and reveal a robust elastohydrodynamic mechanism: the inclusion outpaces the vesicle, sustaining a thinning film that drains symmetrically and self-similarly, largely independent of initial shape. For soft membranes and small inclusions, coupling drives a monotonic tension increase that can exceed the lysis tension. Evaluating the maximal tension over a delivery distance, we map an operating window in vesicle reduced area and size relative to the inclusion.

cond-mat.soft↗

Size Amplification of Jet Drops due to Insoluble Surfactants

Surface bubbles in the environment or engineering configurations, such as the ocean-atmosphere interface, sparkling wine, or during volcanic eruptions typically live on contaminated surfaces. A particularly common type of contamination is surface active agents (surfactants). We consider the effect of insoluble surfactant on jet drop formation by bubble bursting. Contrary to the observed trend that surfactants decrease the ejected drop radius for bubbles with precursor capillary waves, we find that surfactants increase the ejected drop radius for bubbles without precursor capillary waves - a regime characteristic of small bubbles. Consequently, the results have fundamental implications for understanding aerosol distributions in contaminated conditions. We find that the trend reversal is due to the effect of Marangoni stresses on the focusing of the collapsing cavity. We demonstrate quantitative agreement on the jet velocity and drop size between laboratory experiments and numerical simulations by using the measured surface tension dependence on surfactant concentration as the equation of state for the simulations. *Jun Eshima and Tristan Aurégan contributed equally to this work.

physics.flu-dyn↗

Autophoretic skating along permeable surfaces

The dynamics of self-propelled colloidal particles are strongly influenced by their environment through hydrodynamic and, in many cases, chemical interactions. We develop a theoretical framework to describe the motion of confined active particles by combining the Lorentz reciprocal theorem with a Galerkin discretisation of surface fields, yielding an equation of motion that efficiently captures self-propulsion without requiring an explicit solution for the bulk fluid flow. Applying this framework, we identify and characterise the long-time behaviours of a Janus particle near rigid, permeable, and fluid-fluid interfaces, revealing distinct motility regimes, including surface-bound skating, stable hovering, and chemo-hydrodynamic reflection. Our results demonstrate how the solute permeability and the viscosity contrast of the surface influence a particle's dynamics, providing valuable insights into experimentally relevant guidance mechanisms for autophoretic particles. The computational efficiency of our method makes it particularly well-suited for systematic parameter sweeps, offering a powerful tool for mapping the phase space of confined active particles and informing high-fidelity numerical simulations.

physics.flu-dyn↗

Revealing Actual Viscoelastic Relaxation Times in Capillary Breakup

We use experiments and theory to elucidate the size effect in capillary breakup rheometry, where pre-stretching in the visco-capillary stage causes the apparent relaxation time to be consistently smaller than the actual value. We propose a method accounting for both the experimental size and the finite extensibility of polymers to extract the actual relaxation time. A phase diagram characterizes the expected measurement variability and delineates scaling law conditions. The results refine capillary breakup rheometry for viscoelastic fluids and advance the understanding of breakup dynamics across scales.

cond-mat.soft↗

Transient rod-climbing in an Oldroyd-B fluid

The Weissenberg effect, or rod-climbing phenomenon, occurs in non-Newtonian fluids where the fluid interface ascends along a rotating rod. Despite its prominence, theoretical insights into this phenomenon remain limited. In earlier work, Joseph \& Fosdick (\emph{Arch. Rat. Mech. Anal.}, vol. 49, 1973, pp. 321--380) employed domain perturbation methods for second-order fluids to determine the equilibrium interface height by expanding solutions based on the rotation speed. In this work, we investigate the time-dependent interface height through asymptotic analysis with dimensionless variables and equations using the Oldroyd-B model. We begin by neglecting surface tension and inertia to focus on the interaction between gravity and viscoelasticity. In the small-deformation scenario, the governing equations indicate the presence of a boundary layer in time, where the interface rises rapidly over a short time scale before gradually approaching a steady state. By employing a stretched time variable, we derive the transient velocity field and corresponding interface profile on this short time scale and recover the steady-state profile on a longer time scale. Subsequently, we reintroduce small but finite inertial effects to investigate their interplay with viscoelasticity and propose a criterion for determining the conditions under which rod-climbing occurs.

physics.flu-dyn↗

Close-contact melting on hydrophobic textured surfaces: Confinement and meniscus effects

We investigate the dynamics of close-contact melting (CCM) on gas-trapped hydrophobic surfaces, with specific focus on the effects of geometrical confinement and the liquid-air meniscus below the liquid film. By employing dual-series and perturbation methods, we obtain numerical solutions for the effective slip lengths associated with velocity $λ$ and temperature $λ_t$ fields, across various values of aspect ratio $Λ$ (defined as the ratio of the film thickness $h$ to the structure's periodic length $l$) and gas-liquid fraction $ϕ$. Asymptotic solutions of $λ$ and $λ_t$ for $Λ\ll 1$ and $Λ\gg 1$ are derived and summarized for different surface structures, interface shapes and $Λ$, which reveal a different trend for $λ$ and $Λ\ll 1$ and the presence of a meniscus. In the context of constant-pressure CCM, our results indicate that transverse-grooves surfaces consistently reduced the heat transfer. However, longitudinal grooves can enhance heat transfer under the effects of confinement and meniscus when $Λ\lessapprox 0.1$ and $ϕ< 1 - 0.5^{2/3} \approx 0.37$. For gravity-driven CCM, the parameters of $l$ and $ϕ$ determine whether the melting rate is enhanced, reduced, or nearly unaffected. We construct a phase diagram based on the parameter matrix $(\log_{10} l, ϕ)$to delineate these three regimes. Lastly, we derived two asymptotic solutions for predicting the variation in time of the unmelted solid height.

cond-mat.soft↗

Surface Furrowing Instability in Everting Soft Solids

We report a surface instability observed during the extrusion of extremely soft elastic solids in confined geometries. Due to their unique rheological properties, these soft solids can migrate through narrow gaps by continuously everting the bulk material. The extrusion front spontaneously buckles in the direction transverse to the flow, resulting in a furrow-like morphology that deepens over time. We characterize the distinct features of this instability using experiments and theory and contrast the results with known elastic surface instabilities. Our study may provide insights into various processes involving the extrusion-like deformations of soft solids, including biomaterials.

cond-mat.soft↗

Hydrodynamics of molecular rotors in lipid membranes

Molecular rotors form twisted conformations upon photoexcitation, with their fluorescent relaxation time serving as a measure of viscosity. They have been used to assess membrane viscosities but yield higher values compared to other methods. Here, we show that the rotor's relaxation time is influenced by a combination of membrane viscosity and interleaflet friction. We present a theory for the relaxation time and obtain a correction factor that accounts for the discrepancy. If the membrane's viscosity is known, molecular rotors may enable the extraction of the elusive interleaflet friction.

cond-mat.soft↗

The 2024 Motile Active Matter Roadmap

Activity and autonomous motion are fundamental aspects of many living and engineering systems. Here, the scale of biological agents covers a wide range, from nanomotors, cytoskeleton, and cells, to insects, fish, birds, and people. Inspired by biological active systems, various types of autonomous synthetic nano- and micromachines have been designed, which provide the basis for multifunctional, highly responsive, intelligent active materials. A major challenge for understanding and designing active matter is their inherent non-equilibrium nature due to persistent energy consumption, which invalidates equilibrium concepts such as free energy, detailed balance, and time-reversal symmetry. Furthermore, interactions in ensembles of active agents are often non-additive and non-reciprocal. An important aspect of biological agents is their ability to sense the environment, process this information, and adjust their motion accordingly. It is an important goal for the engineering of micro-robotic systems to achieve similar functionality. With many fundamental properties of motile active matter now reasonably well understood and under control, the ground is prepared for the study of physical aspects and mechanisms of motion in complex environments, of the behavior of systems with new physical features like chirality, of the development of novel micromachines and microbots, of the emergent collective behavior and swarming of intelligent self-propelled particles, and of particular features of microbial systems. The vast complexity of phenomena and mechanisms involved in the self-organization and dynamics of motile active matter poses major challenges, which can only be addressed by a truly interdisciplinary effort involving scientists from biology, chemistry, ecology, engineering, mathematics, and physics.

cond-mat.soft↗

On the self-similarity of unbounded viscous Marangoni flows

The Marangoni flow induced by an insoluble surfactant on a fluid-fluid interface is a fundamental problem investigated extensively due to its implications in colloid science, biology, the environment, and industrial applications. Here, we study the limit of a deep liquid subphase with negligible inertia (low Reynolds number, $Re\ll{1}$), where the two-dimensional problem has been shown to be described by the complex Burgers equation. We analyze the problem through a self-similar formulation, providing further insights into its structure and revealing its universal features. Six different similarity solutions are found. One of the solutions includes surfactant diffusion, whereas the other five, which are identified through a phase-plane formalism, hold only in the limit of negligible diffusion (high surface Péclet number $Pe_s\gg{1}$). Surfactant 'pulses', with a locally higher concentration that spreads outward, lead to two similarity solutions of the first kind with a similarity exponent $β=1/2$. On the other hand, distributions that are locally depleted and flow inwards lead to similarity of the second kind, with two different exponents that we obtain exactly using stability arguments. We distinguish between 'dimple' solutions, where the surfactant has a quadratic minimum and $β=2$, from 'hole' solutions, where the concentration profile is flatter than quadratic and $β=3/2$. Each of these two cases exhibits two similarity solutions, one earlier than a critical time $t_*$ when the derivative of the concentration is singular, and another one valid after $t_*$. We obtain all six solutions in closed form, and discuss predictions that can be extracted from these results.

physics.flu-dyn↗

Deformation Dynamics of Nanopores upon Water Imbibition

Capillarity-driven transport in nanoporous solids is widespread in nature and crucial for modern liquid-infused engineering materials. During imbibition, curved menisci driven by high negative Laplace pressures exert an enormous contractile load on the porous matrix. Due to the challenge of simultaneously monitoring imbibition and deformation with high spatial resolution, the resulting coupling of solid elasticity to liquid capillarity has remained largely unexplored. Here, we study water imbibition in mesoporous silica using optical imaging, gravimetry, and high-resolution dilatometry. In contrast to an expected Laplace pressure-induced contraction, we find a square-root-of-time expansion and an additional abrupt length increase when the menisci reach the top surface. The final expansion is absent when we stop the imbibition front inside the porous medium in a dynamic imbibition-evaporation equilibrium, as is typical for transpiration-driven hydraulic transport in plants, especially in trees. These peculiar deformation behaviors are validated by single-nanopore molecular dynamics simulations and described by a continuum model that highlights the importance of expansive surface stresses at the pore walls (Bangham effect) and the buildup or release of contractile Laplace pressures as menisci collectively advance, arrest, or disappear. Our model suggests that these observations apply to any imbibition process in nanopores, regardless of the liquid/solid combination, and that the Laplace contribution upon imbibition is precisely half that of vapor sorption, due to the linear pressure drop associated with viscous flow. Thus, simple deformation measurements can be used to quantify surface stresses and Laplace pressures or transport in a wide variety of natural and artificial porous media.

cond-mat.soft↗

Viscoelastic fluid flow in a slowly varying planar contraction: the role of finite extensibility on the pressure drop

We analyze the steady viscoelastic fluid flow in slowly varying contracting channels of arbitrary shape and present a theory based on the lubrication approximation for calculating the flow rate-pressure drop relation at low and high Deborah ($De$) numbers. Unlike most prior theoretical studies leveraging the Oldroyd-B model, we describe the fluid viscoelasticity using a FENE-CR model and examine how the polymer chains' finite extensibility impacts the pressure drop. We employ the low-Deborah-number lubrication analysis to provide analytical expressions for the pressure drop up to $O(De^4)$. We further consider the ultra-dilute limit and exploit a one-way coupling between the parabolic velocity and elastic stresses to calculate the pressure drop of the FENE-CR fluid for arbitrary values of the Deborah number. Such an approach allows us to elucidate elastic stress contributions governing the pressure drop variations and the effect of finite extensibility for all $De$. We validate our theoretical predictions with two-dimensional numerical simulations and find excellent agreement. We show that, at low Deborah numbers, the pressure drop of the FENE-CR fluid monotonically decreases with $De$, similar to the previous results for the Oldroyd-B and FENE-P fluids. However, at high Deborah numbers, in contrast to a linear decrease for the Oldroyd-B fluid, the pressure drop of the FENE-CR fluid exhibits a non-monotonic variation due to finite extensibility, first decreasing and then increasing with $De$. Nevertheless, even at sufficiently high Deborah numbers, the pressure drop of the FENE-CR fluid in the ultra-dilute and lubrication limits is lower than the corresponding Newtonian pressure drop.

physics.flu-dyn↗

Exact Analytical Solution of the Flory-Huggins Model and Extensions to Multicomponent Systems

The Flory-Huggins theory describes the phase separation of solutions containing polymers. Although it finds widespread application from polymer physics to materials science to biology, the concentrations that coexist in separate phases at equilibrium have not been determined analytically, and numerical techniques are required that restrict the theory's ease of application. In this work, we derive an implicit analytical solution to the Flory-Huggins theory of one polymer in a solvent by applying a procedure that we call the implicit substitution method. While the solutions are implicit and in the form of composite variables, they can be mapped explicitly to a phase diagram in composition space. We apply the same formalism to multicomponent polymeric systems, where we find analytical solutions for polydisperse mixtures of polymers of one type. Finally, while complete analytical solutions are not possible for arbitrary mixtures, we propose computationally efficient strategies to map out coexistence curves for systems with many components of different polymer types.

cond-mat.soft↗

Triboelectrically mediated self-assembly and manipulation of drops at an interface

The fluid-fluid interface is a complex environment for a floating object where the statics and dynamics may be governed by capillarity, gravity, inertia, and other external body forces. Yet, the alignment of these forces in intricate ways might result in beautiful pattern formation and self-assembly of these objects, as in the case of bubble rafts or colloidal particles. While interfacial self-assembly has been explored widely, controlled manipulation of floating objects, e.g. drops, at the fluid-fluid interface still remains a challenge largely unexplored. In this work, we reveal the self-assembly and manipulation of water drops floating at an oil-air interface. We show that the assembly occurs due to electrostatic interactions between the drops and their environment. We highlight the role of the boundary surrounding the system by showing that even drops with a net zero electric charge can self-assemble under certain conditions. Using experiments and theory, we show that the depth of the oil bath plays an important role in setting the distance between the self-assembled drops. Furthermore, we demonstrate ways to manipulate the drops actively and passively at the interface.

physics.flu-dyn↗