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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.

Elastoviscoplastic (EVP) fluids, which exhibit both solid-like and liquid-like behavior depending on the applied stress, are critical in industrial processes involving complex geometries such as porous media and wavy channels. In this study, we investigate how flow characteristics and channel design affect EVP fluid flow through a wavy channel, using numerical simulations supported by microfluidic experiments. Our results reveal that elasticity significantly influences flow dynamics, reducing pressure drops and expanding unyielded regions. Notably, we find that even minimal elasticity can shift the flow from steady to time-dependent regimes, a transition less pronounced in viscoelastic fluids. Additionally, we show that the development of stagnation regions can be prevented when using a modified EVP fluid with enhanced elasticity, thus providing a full global yielding of the material. This study elucidates the role of elasticity in modifying flow patterns and stress distribution within EVP fluids, offering insights into the optimization of industrial applications, such as the displacement of yield stress fluids in enhanced oil recovery, gas extraction, cementing, and other processes where flow efficiency is critical., Comment: 15 pages, 19 figures

The thinning of liquid bridges under capillary stress occurs in widespread processes like jetting, dripping, and spraying, and creates a strong extensional flow capable of stretching dissolved polymers. If the elastic stress exceeds the viscous stress, an exponential `elastocapillary' (EC) thinning regime arises, yielding a timescale $\tau_{EC}$ commonly considered to be the longest relaxation time of the polymer $\lambda$. A longstanding question is why $\tau_{EC}$ depends on the polymer concentration, even at high dilutions where $\lambda$ should be constant in theory. To date this is understood in terms of intermolecular interactions that arise as polymers stretch. However, we show how the concentration dependence of $\tau_{EC}$ can be explained by considering the molecular weight distribution (MWD) inherent in real polymer samples. We demonstrate this by blending low-$M$ and high-$M$ polymer samples with narrow MWDs at dilute concentrations and in different proportions, and by measuring $\tau_{EC}$ for each blend in capillary thinning experiments. A simple model qualitatively reproduces the experimental results, showing how elastic stresses generated by the polymer build up prior to the EC regime due to sequential stretching of decreasing molecular weight species in the MWD. Since the elastic stress generated by each species depends on its concentration, the fraction of the MWD that is required to stretch in order to induce the EC regime depends on the total polymer concentration $c$. For higher $c$ the EC regime is induced by stretching of a higher-$M$ (longer $\lambda$) fraction of the MWD, and results in a longer measurement of $\tau_{EC}$. Our results have significant implications for the application of capillary thinning measurements to extensional rheometry, for the interpretation of such measurements, and for the understanding of elastocapillary thinning dynamics in general., Comment: 15 pages, 8 figures, 1 table, 3 supplementary figures

In this study, we delve into the intricacies of elastoviscoplastic (EVP) fluids, particularly focusing on how polymer additives influence their extensional behavior. Our findings reveal that polymer additives significantly alter the extensional properties of the EVP fluids, such as relaxation time and extensional stresses, while having negligible impact on the shear rheology. Interestingly, the modified fluids exhibit a transition from yield stress-like behavior to viscoelastic-like behavior under high extensional rates, ultimately leading to destabilization under extreme deformation. This research enhances the fundamental understanding of EVP fluids and highlights potential advancements in applications, especially in precision-demanding fields like 3D printing., Comment: 20 pages, 15 figures

Measurements of the capillary-driven thinning and breakup of fluid filaments are widely used to extract extensional rheological properties of complex materials. For viscoelastic (e.g., polymeric) fluids, the determination of the longest relaxation time depends on several assumptions concerning the polymeric response to the flow that are derived from constitutive models. Our capillary thinning experiments using polymeric fluids with a wide range of extensibility, suggest that these assumptions are likely only valid for highly extensible polymers but do not hold in general. For polymers with relatively low extensibility, such as polyectrolytes in salt-free media, conventional extrapolation of the longest relaxation time from capillary thinning techniques leads to a significant underestimation.

Polymers and rod-like colloids (PaRC) adopt a favorable orientation under sufficiently strong flows. However, how the flow kinematics affect the alignment of such nanostructures according to their extensibility remains unclear. By analysing the shear- and extension-induced alignment of chemically and structurally different PaRC, we show that extensibility is a key determinant of the structural response to the imposed kinematics. We propose a unified description of the effectiveness of extensional flow, compared to shearing flow, at aligning PaRC of different extensibility.

In Part I of this paper [Haward et al. submitted (2023)], we presented a new three-dimensional microfluidic device (the optimized uniaxial and biaxial extensional rheometer, OUBER) for generating near-homogeneous uniaxial and biaxial elongational flows. In this Part II of the paper, we employ the OUBER device to examine the uniaxial and biaxial extensional rheology of some model dilute polymer solutions. We also compare the results with measurements made under planar extension in the optimized-shape cross-slot extensional rheometer [or OSCER, Haward et al. Phys. Rev. Lett. (2012)]. In each case (uniaxial, planar and biaxial extension), we use micro-particle image velocimetry to measure the extension rate as a function of the imposed flow rate, and we measure the excess pressure drop across each device in order to estimate the tensile stress difference generated in the fluid. We present a new analysis, based on solving the macroscopic power balance for flow through each device, to refine the estimate of the tensile stress difference obtained from the measured pressure drop. Based on this analysis, we find that for our most dilute polymer sample, which is "ultradilute", the extensional viscosity is well described by the finitely extensible non-linear elastic dumbbell model. In this limit, the biaxial extensional viscosity at high Weissenberg numbers (Wi) is half that of the uniaxial and planar extensional viscosities. At higher polymer concentrations, the experimental measurements deviate from the model predictions, which is attributed to the onset of intermolecular interactions as polymers unravel in the extensional flows. Of practical significance (and fundamental interest), elastic instability occurs at a significantly lower Wi in uniaxial extensional flow than in either biaxial or planar extensional flow, limiting the utility of this flow type for extensional viscosity measurement.

We present a numerical optimization of a "6-arm cross-slot" device, yielding several three-dimensional shapes of fluidic channels designed to impose close approximations to ideal uniaxial (or biaxial) stagnation point extensional flow under the constraints of having four inlets and two outlets (or two inlets and four outlets) and Newtonian creeping flow conditions. Of the various numerically-generated geometries, one is selected as being most suitable for fabrication at the microscale, and numerical simulations with the Oldroyd-B and Phan-Thien and Tanner models confirm that the optimal flow fields in the chosen geometry are observed for both constant viscosity and shear thinning viscoelastic fluids. Fabrication of the geometry, which we name the optimized uniaxial and biaxial extensional rheometer (OUBER), is achieved with high precision at the microscale by selective laser-induced etching of a fused-silica substrate. Employing a viscous Newtonian fluid with a refractive index matched to that of the optically transparent microfluidic device, we conduct microtomographic-particle image velocimetry in order to resolve the flow field at low Reynolds number (< 0.1) in a substantial volume around the stagnation point. The flow velocimetry confirms the accurate imposition of the desired and predicted flows, with pure extensional flow at an essentially uniform deformation rate being applied over a wide region around the stagnation point. In Part II of this paper [Haward et al., J. Rheol. submitted (2023)], pressure drop measurements in the OUBER geometry will be used to assess the uniaxial and biaxial extensional rheometry of dilute polymeric solutions, in comparison to measurements made in planar extension using an optimized-shape cross-slot extensional rheometer (OSCER, Haward et al, Phys. Rev. Lett., 2012).

In a viscoelastic flow over a microfluidic canopy of polymeric pillars, we report the spontaneous emergence of waves in the form of propagating regions of low flow velocity compared to the surrounding flow. The occurrence of the wave is chaotic and shows characteristics of elastic turbulence. We systematically study the coupling between the low velocity wave and the microfluidic canopy by combining flow velocimetry experiments and high speed tracking of the pillars. The waves form an angle $\beta$ with the primary flow direction that depends on the geometry of the pillar array. If the canopy is composed of flexible structures, the passage of a wave deflects the structures locally in a manner reminiscent of the emergence of the Monami waves observed in inertial turbulence over canopies of vegetation. Due to the analogies with classical (inertial) canopy turbulence, we name our newly-observed phenomenon as canopy elastic turbulence., Comment: 15 pages, 12 figures

Understanding the hydrodynamic alignment of colloidal rods in polymer solutions is pivotal for manufacturing structurally ordered materials. How polymer crowding influences the flow-induced alignment of suspended colloidal rods remains unclear when rods and polymers share similar length-scales. We tackle this problem by analyzing the alignment of colloidal rods suspended in crowded polymer solutions, and comparing against the case where crowding is provided by additional colloidal rods in a pure solvent. We find that the polymer dynamics govern the onset of shear-induced alignment of colloidal rods suspended in polymer solutions, and the control parameter for the alignment of rods is the Weissenberg number, quantifying the elastic response of the polymer to an imposed flow. Moreover, we show that the increasing colloidal alignment with the shear rate follows a universal trend that is independent of the surrounding crowding environment. Our results indicate that colloidal rod alignment in polymer solutions can be predicted based on the critical shear rate at which polymer coils are deformed by the flow, aiding the synthesis and design of anisotropic materials., Comment: 29 pages, 6 figures, under consideration in Macromolecules

Viscoelastic fluids are a common subclass of rheologically complex materials that are encountered in diverse fields from biology to polymer processing. Often the flows of viscoelastic fluids are unstable in situations where ordinary Newtonian fluids are stable, owing to the nonlinear coupling of the elastic and viscous stresses. Perhaps more surprisingly, the instabilities produce flows with the hallmarks of turbulence -- even though the effective Reynolds numbers may be $O(1)$ or smaller. We provide perspectives on viscoelastic flow instabilities by integrating the input from speakers at a recent international workshop: historical remarks, characterization of fluids and flows, discussion of experimental and simulation tools, and modern questions and puzzles that motivate further studies of this fascinating subject. The materials here will be useful for researchers and educators alike, especially as the subject continues to evolve in both fundamental understanding and applications in engineering and the sciences., Comment: A perspective article based on a virtual workshop of the Princeton Center for Theoretical Sciences that took place in January 2021

Viscoelastic flows through porous media become unstable and chaotic beyond critical flow conditions, impacting industrial and biological processes. Recently, Walkama \textit{et al.} [Phys. Rev. Lett. \textbf{124}, 164501 (2020)] have shown that geometric disorder greatly suppresses such chaotic dynamics. We demonstrate experimentally that geometric disorder \textit{per se} is not the reason for this suppression, and that disorder can also promote choatic fluctuations, given a slightly modified initial condition. The results are explained by the effect of disorder on the occurrence of stagnation points exposed to the flow field, which depends on the initially ordered geometric configuration.

Viscoelastic flow through an abrupt planar contraction geometry above a certain Weissenberg number (Wi) is well known to become unstable upstream of the contraction plane via a central jet separating from the walls and forming vortices in the salient corners. Here, for the first time we consider three-dimensional (3D) viscoelastic contraction flows in a microfabricated glass square-square contraction geometry. We employ state-of-the-art microtomographic particle image velocimetry to produce time-resolved and volumetric quantification of the 3D viscoelastic instabilities arising in a dilute polymer solution driven through the geometry over a wide range of Wi but at negligible Reynolds number. Based on our observations, we describe new insights into the growth, propagation, and transient dynamics of an elastic vortex formed upstream of the 3D micro-contraction due to flow jetting towards the contraction. At low Wi we observe vortex growth for increasing Wi, followed by a previously unreported vortex growth plateau region. In the plateau region, the vortex circulates around the jet with a period that decreases with Wi but an amplitude that is independent of Wi. In addition, we report new out-of-plane asymmetric jetting behaviour with a phase-wise dependence on Wi. Finally, we resolve the rate-of-strain tensor D and ascribe local gradients in D as the underlying driver of circulation via strain-hardening of the fluid in the wake of the jet.

Viscoelastic flows through microscale porous arrays exhibit complex path-selection and switching phenomena. However, understanding this process is limited by a lack of studies linking between a single object and large arrays. Here, we report experiments on viscoelastic flow past side-by-side microcylinders with variable intercylinder gap. With increasing flow rate, a sequence of two imperfect symmetry-breaking bifurcations forces selection of either one or two of the three possible flow paths around the cylinders. Tuning the gap length through the value where the first bifurcation becomes perfect reveals regions of bi and tristability in a dimensionless flow rate-gap length `phase' diagram., Comment: 5 pages, 4 figures

Cellulose nanocrystals (CNC) can be considered as model colloidal rods and have practical applications in the formation of soft materials with tailored anisotropy. Here, we employ two contrasting microfluidic devices to quantitatively elucidate the role of shearing and extensional flows on the alignment of a dilute CNC dispersion. Characterization of the flow field by micro-particle image velocimetry is coupled to flow-induced birefringence analysis to quantify the deformation rate--alignment relationship. The deformation rate required for CNC alignment is 4$\times$ smaller in extension than in shear. Alignment in extension is independent of the deformation rate magnitude, but is either 0$^\circ$ or 90$^\circ$ to the flow, depending on its sign. In shear flow the colloidal rods orientate progressively towards 0$^\circ$ as the deformation rate magnitude increases. Our results decouple the effects of shearing and extensional kinematics at aligning colloidal rods, establishing coherent guidelines for the manufacture of structured soft materials.

Secondary flows are ubiquitous in channel flows, where small velocity components perpendicular to the main velocity appear due to the complexity of the channel geometry and/or that of the flow itself such as from inertial or non-Newtonian effects, etc. We investigate here the inertialess secondary flow of viscoelastic fluids in curved microchannels of rectangular cross-section and constant but alternating curvature: the so-called "serpentine channel" geometry. Numerical calculations (Poole et al, 2013) have shown that in this geometry, in the absence of elastic instabilities, a steady secondary flow develops that takes the shape of two counter-rotating vortices in the plane of the channel cross-section. We present the first experimental visualization evidence and characterization of these steady secondary flows, using a complementarity of microPIV in the plane of the channel, and confocal visualisation of dye-stream transport in the cross-sectional plane. We show that the measured streamlines and the relative velocity magnitude of the secondary flows are in qualitative agreement with the numerical results. In addition to our techniques being broadly applicable to the characterisation of three-dimensional flow structures in microchannels, our results are important for understanding the onset of instability in serpentine viscoelastic flows., Comment: This is a post-peer-review, pre-copyedit version of an article published in Microfluidics and Nanofluidics. The final authenticated version is available online at: http://dx.doi.org/10.1007/s10404-019-2195-0

3D-printed microfluidic devices offer new ways to study fluid dynamics. We present the first clear visualization of vortex breakdown in a dividing T-junction flow. By individual control of the inflow and two outflows, we decouple the effects of swirl and rate of vorticity decay. We show that even slight outflow imbalances can greatly alter the structure of vortex breakdown, by creating a net pressure difference across the junction. Our results are summarized in a dimensionless phase diagram, which will guide the use of vortex breakdown in T-junctions to achieve specific flow manipulation., Comment: 5 pages, 5 figures

Experimental measurements and numerical simulations are made on fluid flow through cross-slot devices with a range of aspect (depth:width) ratios, 0.4 < alpha < 3.87. For low Reynolds numbers Re, the flow is symmetric and a sharp boundary exists between fluid streams entering the cross-slot from opposite directions. Above an alpha-dependent critical value Re_c, the flow undergoes a symmetry-breaking bifurcation (though remains steady and laminar) and a spiral vortex structure develops about the central axis of the outflow channel. An order parameter characterizing the instability grows according to a sixth-order Landau potential, and shows a progression from second order to first order transitions as alpha increases. A tricritical point occurs for alpha ~ 0.55. The spiral vortex acts as a mixing region in the flow field and this phenomenon can be used to drive enhanced mixing in microfluidic devices.