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Christopher A. Browne

Publications and source records attributed to Christopher A. Browne.

13 recordsLinked to original sources

Arrested coalescence drives helical coiling and networking of filamentous smectic condensates

Liquid-liquid crystal phase separation (LLCPS) occurs in many industrial and biological settings. Interestingly, when smectic phases demix from the homogeneous mixture, they can form filamentous condensates that spontaneously assemble into sparse networks with rich life-like dynamics. Here, we study the underlying process of filament networking. Microscopy reveals that new linkages between filaments are initiated by an adhesive interaction between straight filaments; parallel filaments snap into contact and then rapidly wind into helical coils, despite the absence of molecular chirality or transitions between mesophases. Using polarized optical microscopy, theoretical modeling, and simulation, we show that parallel filaments coalesce, but are arrested in double-barreled ``ribbon'' structures. This arrested coalescence is driven purely by interfacial energy minimization under the constraints of smectic layering. The arrested ribbons spontaneously coil into double helices to further reduce interfacial area, thus driving compaction into networks. We propose a microstructure consistent with this interpretation, which quantitatively predicts the extent of arrested coalescence. In total, these findings suggest a generic pathway for network formation in liquid crystals that provides insight about the formation of condensate networks in other engineered or biological materials.

cond-mat.soft

Getting out of a tight spot: Cooperative unclogging of hydrogel particles in disordered porous media

We use event-driven pore network modeling to study the transport of hydrogel particles through disordered porous media -- a process that underlies diverse applications. By simulating particle advection, deformation, and clogging at the pore scale, we identify a dimensionless "squeezing parameter" that quantitatively predicts the depth to which particles penetrate into a given medium across diverse conditions. Our simulations also uncover a surprising cooperative effect: adding more particles enables them to penetrate deeper into the medium. This phenomenon arises because individual particles redirect fluid to adjacent throats, forcing nearby particles through tight pores that they would otherwise clog. Altogether, these results help to establish a quantitative framework that connects microscopic particle mechanics to macroscopic transport behavior.

cond-mat.soft

Stagnation points at grain contacts generate an elastic flow instability in 3D porous media

Many environmental, energy, and industrial processes involve the flow of polymer solutions in three-dimensional (3D) porous media where fluid is confined to navigate through complex pore space geometries. As polymers are transported through the tortuous pore space, elastic stresses accumulate, leading to the onset of unsteady flow fluctuations above a threshold flow rate. How does pore space geometry influence the development and features of this elastic instability? Here, we address this question by directly imaging polymer solution flow in microfabricated 3D ordered porous media with precisely controlled geometries consisting of simple-cubic (SC) or body-centered cuboid (BC) arrays of spherical grains. In both cases, we find that the flow instability is generated at stagnation points arising at the contacts between grains rather than at the polar upstream/downstream grain surfaces, as is the case for flow around a single grain. The characteristics of the flow instability are strongly dependent on the unit cell geometry: in SC packings, the instability manifests through the formation of time-dependent, fluctuating 3D eddies, whereas in BC packings, it manifests as continual fluctuating 'wobbles' and crossing in the flow pathlines. Despite this difference, we find that characteristics of the transition from steady to unsteady flow with increasing flow rate have commonalities across geometries. Moreover, for both packing geometries, our data indicate that extensional flow-induced polymeric stresses generated by contact-associated stagnation points are the primary contributor to the macroscopic resistance to flow across the entire medium. Altogether, our work highlights the pivotal role of inter-grain contacts -- which are typically idealized as discrete points and therefore overlooked, but are inherent in most natural and engineered media -- in shaping elastic instabilities in porous media.

physics.flu-dyn

Spontaneous assembly of condensate networks during the demixing of structured fluids

Liquid-liquid phase separation, whereby two liquids spontaneously demix, is ubiquitous in industrial, environmental, and biological processes. While isotropic fluids are known to condense into spherical droplets in the binodal region, these dynamics are poorly understood for structured fluids. Here, we report the novel observation of condensate networks, which spontaneously assemble during the demixing of a mesogen from a solvent. Condensing mesogens form rapidly-elongating filaments, rather than spheres, to relieve distortion of a simultaneously-forming internal smectic mesophase. As filaments densify, they collapse into bulged discs, lowering the elastic free energy. Additional distortion is relieved by retraction of filaments into the bulged discs, which are straightened under tension to form a ramified network. Understanding and controlling these dynamics may provide new avenues to direct pattern formation or template materials.

cond-mat.soft

Harnessing elastic instabilities for enhanced mixing and reaction kinetics in porous media

Turbulent flows have been used for millennia to mix solutes; a familiar example is stirring cream into coffee. However, many energy, environmental, and industrial processes rely on the mixing of solutes in porous media where confinement suppresses inertial turbulence. As a result, mixing is drastically hindered, requiring fluid to permeate long distances for appreciable mixing and introducing additional steps to drive mixing that can be expensive and environmentally harmful. Here, we demonstrate that this limitation can be overcome just by adding dilute amounts of flexible polymers to the fluid. Flow-driven stretching of the polymers generates an elastic instability (EI), driving turbulent-like chaotic flow fluctuations, despite the pore-scale confinement that prohibits typical inertial turbulence. Using in situ imaging, we show that these fluctuations stretch and fold the fluid within the pores along thin layers (``lamellae'') characterized by sharp solute concentration gradients, driving mixing by diffusion in the pores. This process results in a $3\times$ reduction in the required mixing length, a $6\times$ increase in solute transverse dispersivity, and can be harnessed to increase the rate at which chemical compounds react by $3\times$ -- enhancements that we rationalize using turbulence-inspired modeling of the underlying transport processes. Our work thereby establishes a simple, robust, versatile, and predictive new way to mix solutes in porous media, with potential applications ranging from large-scale chemical production to environmental remediation.

physics.flu-dyn

Fluid drainage in erodible porous media

Drainage, in which a nonwetting fluid displaces a wetting fluid from a porous medium, is well-studied for media with unchanging solid surfaces. However, many media can be eroded by drainage, with eroded material redeposited in pores downstream, altering further flow. Here, we use theory and simulation to examine how these coupled processes both alter the overall fluid displacement pathway and help reshape the solid medium. We find two new drainage behaviors with markedly different characteristics, and quantitatively delineate the conditions under which they arise. Our results thereby help expand current understanding of these rich physics, with implications for applications of drainage in industry and the environment.

physics.flu-dyn

Elastic turbulence homogenizes fluid transport in stratified porous media

Many key environmental, industrial, and energy processes rely on controlling fluid transport within subsurface porous media. These media are typically structurally heterogeneous, often with vertically-layered strata of distinct permeabilities -- leading to uneven partitioning of flow across strata, which can be undesirable. Here, using direct in situ visualization, we demonstrate that polymer additives can homogenize this flow by inducing a purely-elastic flow instability that generates random spatiotemporal fluctuations and excess flow resistance in individual strata. In particular, we find that this instability arises at smaller imposed flow rates in higher-permeability strata, diverting flow towards lower-permeability strata and helping to homogenize the flow. Guided by the experiments, we develop a parallel-resistor model that quantitatively predicts the flow rate at which this homogenization is optimized for a given stratified medium. Thus, our work provides a new approach to homogenizing fluid and passive scalar transport in heterogeneous porous media.

physics.flu-dyn

Infection percolation: A dynamic network model of disease spreading

Models of disease spreading are critical for predicting infection growth in a population and evaluating public health policies. However, standard models typically represent the dynamics of disease transmission between individuals using macroscopic parameters that do not accurately represent person-to-person variability. To address this issue, we present a dynamic network model that provides a straightforward way to incorporate both disease transmission dynamics at the individual scale as well as the full spatiotemporal history of infection at the population scale. We find that disease spreads through a social network as a traveling wave of infection, followed by a traveling wave of recovery, with the onset and dynamics of spreading determined by the interplay between disease transmission and recovery. We use these insights to develop a scaling theory that predicts the dynamics of infection for diverse diseases and populations. Furthermore, we show how spatial heterogeneities in susceptibility to infection can either exacerbate or quell the spread of disease, depending on its infectivity. Ultimately, our dynamic network approach provides a simple way to model disease spreading that unifies previous findings and can be generalized to diverse diseases, containment strategies, seasonal conditions, and community structures.

physics.soc-ph

Elastic turbulence generates anomalous flow resistance in porous media

Diverse processes rely on the viscous flow of polymer solutions through porous media. In many cases, the macroscopic flow resistance abruptly increases above a threshold flow rate in a porous medium---but not in bulk solution. The reason why has been a puzzle for over half a century. Here, by directly visualizing the flow in a transparent 3D porous medium, we demonstrate that this anomalous increase is due to the onset of an elastic instability. We establish that the energy dissipated by the unstable flow fluctuations, which vary across pores, generates the anomalous increase in flow resistance through the entire medium. Thus, by linking the pore-scale onset of unstable flow to macroscopic transport, our work provides generally-applicable guidelines for predicting and controlling polymer solution flows.

physics.flu-dyn

Forced Imbibition in Stratified Porous Media

Imbibition plays a central role in diverse energy, environmental, and industrial processes. In many cases, the medium has multiple parallel strata of different permeabilities; however, how this stratification impacts imbibition is poorly understood. We address this gap in knowledge by directly visualizing forced imbibition in three-dimensional (3D) porous media with two parallel strata. We find that imbibition is spatially heterogeneous: for small capillary number Ca, the wetting fluid preferentially invades the fine stratum, while for Ca above a threshold value, the fluid instead preferentially invades the coarse stratum. This threshold value depends on the medium geometry, the fluid properties, and the presence of residual wetting films in the pore space. These findings are well described by a linear stability analysis that incorporates crossflow between the strata. Thus, our work provides quantitative guidelines for predicting and controlling flow in stratified porous media.

physics.flu-dyn

Bistability in the Unstable Flow of Polymer Solutions Through Porous Media

Polymer solutions are often injected in porous media for applications such as oil recovery and groundwater remediation. As the fluid navigates the tortuous pore space, elastic stresses build up, causing the flow to become unstable at sufficiently large injection rates. However, it is poorly understood how the spatial and temporal characteristics of this unstable flow depend on pore space geometry. We elucidate this dependence by systematically varying the spacing between pore constrictions in a model porous medium. We find that when the pore spacing is large, unstable eddies form upstream of each pore, similar to observations of an isolated pore. By contrast, when the pore spacing is sufficiently small, the flow exhibits a surprising bistability, stochastically switching between two distinct unstable flow states. We hypothesize that this unusual behavior arises from the interplay between flow-induced polymer elongation and relaxation of polymers as they are advected through the porous medium. Consistent with this idea, we find that the flow state in a given pore persists for long times. Moreover, we find that the flow state is correlated between neighboring pores; however, these correlations do not persist long-range. Our results thus help to elucidate the rich array of flow behaviors that can arise in polymer solution flow through porous media.

cond-mat.soft

Pore-Scale Flow Characterization of Polymer Solutions in Microfluidic Porous Media

Polymer solutions are frequently used in enhanced oil recovery and groundwater remediation to improve the recovery of trapped non-aqueous fluids. However, applications are limited by an incomplete understanding of the flow in porous media. The tortuous pore structure imposes both shear and extension, which elongates polymers; moreover, the flow is often at large Weissenberg numbers Wi at which polymer elasticity in turn strongly alters the flow. This dynamic elongation can even produce flow instabilities with strong spatial and temporal fluctuations despite the low Reynolds number Re. Unfortunately, macroscopic approaches are limited in their ability to characterize the pore-scale flow. Thus, understanding how polymer conformations, flow dynamics, and pore geometry together determine these non-trivial flow patterns and impact macroscopic transport remains an outstanding challenge. Here, we describe how microfluidic tools can shed light on the physics underlying the flow of polymer solutions in porous media at high Wi and low Re. Specifically, microfluidic studies elucidate how steady and unsteady flow behavior depends on pore geometry and solution properties, and how polymer-induced effects impact non-aqueous fluid recovery. This work provides new insights for polymer dynamics, non-Newtonian fluid mechanics, and applications such as enhanced oil recovery and groundwater remediation.

cond-mat.soft

Controlling capillary fingering using pore size gradients in disordered media

Capillary fingering is a displacement process that can occur when a non-wetting fluid displaces a wetting fluid from a homogeneous disordered porous medium. Here, we investigate how this process is influenced by a pore size gradient. Using microfluidic experiments and computational pore-network models, we show that the non-wetting fluid displacement behavior depends sensitively on the direction and the magnitude of the gradient. The fluid displacement depends on the competition between a pore size gradient and pore-scale disorder; indeed, a sufficiently large gradient can completely suppress capillary fingering. By analyzing capillary forces at the pore scale, we identify a non-dimensional parameter that describes the physics underlying these diverse flow behaviors. Our results thus expand the understanding of flow in complex porous media, and suggest a new way to control flow behavior via the introduction of pore size gradients.

cond-mat.soft