Gareth H. McKinley

Massachusetts Institute of Technology | MIT · Department of Mechanical Engineering

We perform simulations of an impulsively started, axisymmetric viscoelastic jet exiting a nozzle and entering a stagnant gas phase using the open-source code Basilisk. This code allows for efficient computations through an adaptively refined volume-of-fluid technique that can accurately capture the deformation of the liquid–gas interface. We use th...

Semi-flexible polyelectrolytes are a group of biopolymers with a wide range of applications from drag reducing agents in turbulent flows to thickening agents in food and cosmetics. In this study, we investigate the rheology of aqueous solutions of xanthan gum as a canonical semi-flexible polyelectrolyte in steady shear and transient extensional flo...

Extensional flows of complex fluids play an important role in many industrial applications, such as spraying and atomisation, as well as microfluidic-based drop deposition. The Dripping-on-Substrate (DoS) technique is a...

We study the local dynamics of a thixotropic yield stress fluid that shows a pronounced non-monotonic flow curve. This mechanically unstable behavior is generally not observable from standard rheometry tests,...

Aluminosilicate hydrogels are often considered as precursors for the crystallisation of zeolites carried out under hydrothermal conditions. The preparation of mechanically homogeneous aluminosilicate gels enables the study of these materials...

Gels made of telechelic polymers connected by reversible cross-linkers are a versatile design platform for biocompatible viscoelastic materials. Their linear response to a step strain displays a fast, near-exponential relaxation when using low-valence cross-linkers, while larger supramolecular cross-linkers bring about much slower dynamics involvin...

It is well known that inertia-free shearing flows of a viscoelastic fluid with curved streamlines, such as the torsional flow between a rotating cone and plate or the flow in a Taylor–Couette geometry, can become unstable to a three-dimensional time-dependent instability at conditions exceeding a critical Weissenberg ( $Wi$ ) number. However, the c...

Knowledge of the evolution in the mechanical properties of a curing polymer matrix is of great importance in composite parts or structure fabrication. Conventional rheometry, based on small amplitude oscillatory shear, is limited by long interrogation times. In rapidly evolving materials, time sweeps can provide a meaningful measurement albeit at a...

Laun's rule [H. M. Laun, “Prediction of elastic strains of polymer melts in shear and elongation,” J. Rheol. 30, 459–501 (1986).] is commonly used for evaluating the rate-dependent first normal stress coefficient from the frequency dependence of the complex modulus. We investigate the mathematical conditions underlying the validity of Laun's relati...

The design of soft magnetic hydrogels with high concentrations of magnetic particles is complicated by weak retention of the iron oxide particles in the hydrogel scaffold. Here, we propose a design strategy that circumvents this problem through the in situ mineralization of iron oxide nanoparticles within polymer hydrogels functionalized with stron...

Viscoelastic stress relaxation is a basic characteristic of soft matter systems such as colloids, gels, and biological networks. Although the Maxwell model of linear viscoelasticity provides a classical description of stress relaxation, it is often not sufficient for capturing the complex relaxation dynamics of soft matter. In this Tutorial, we int...

Addition of particles to a viscoelastic suspension dramatically alters the properties of the mixture, particularly when it is sheared or otherwise processed. Shear-induced stretching of the polymers results in elastic stress that causes a substantial increase in measured viscosity with increasing shear, and an attractive interaction between particl...

Saltwater taffy, an American confection consisting of the main ingredients sugar, corn syrup, water, and oil, is known for its chewy texture and diverse flavors. We use a small amplitude oscillatory shear test to probe the linear viscoelastic properties of commercial taffy. At low frequencies, self-similar relaxation behavior characteristic of a cr...

Clay slurries are both ubiquitous and essential in the oil exploration industry, and are most commonly employed as drilling fluids. Due to its natural abundance, bentonite clay is often the de facto choice for these materials. Understanding and predicting the mechanical response of these fluids is critical for safe and efficient drilling operations...

Anticipating qualitative changes in the rheological response of complex fluids (e.g., a gelation or vitrification transition) is an important capability for processing operations that utilize such materials in real-world environments. One class of complex fluids that exhibits distinct rheological states are soft glassy materials such as colloidal g...

We report here the first studies of the electrorheological (ER) effect in a liquid-liquid emulsion, which is composed of a silicone oil and a chlorinated paraffin oil, with a thousand-fold difference between the bulk conductivities of the two components. Transient response of the viscous shear stress exerted by the emulsion is examined following st...

Part I of this paper [Haward et al., J. Rheol. 67, 995–1009 (2023)] presents a three-dimensional microfluidic device (the optimized uniaxial and biaxial extensional rheometer, OUBER) for generating near-homogeneous uniaxial and biaxial elongational flows. Here, in Part II, the OUBER device is employed to examine the uniaxial and biaxial extensional...

Soft biological tissues exhibit a remarkable resilience to large mechanical loads, a property which is associated with the strain stiffening capability of the biopolymer networks that structurally support the tissues. Yet, recent studies have shown that composite systems such as tissues and blood clots exhibit mechanical properties that contradict...

The formulation of rheological constitutive equations-models that relate internal stresses and deformations in complex fluids-is a critical step in the engineering of systems involving soft materials. While data-driven models provide accessible alternatives to expensive first-principles models and less accurate empirical models in many engineering...

The vane-in-cup (VIC) geometry has been widely used for the rheological characterization of yield-stress fluids because it minimizes slip effects at the liquid/solid interface of the rotating geometry and reduces sample damage during the loading process. However, severe kinematic limitations arising from the spatial complexity of mixed shear and ex...

The interplay between viscoelasticity and inertia in dilute polymer solutions at high deformation rates can result in inertioelastic instabilities. The nonlinear evolution of these instabilities generates a state of turbulence with significantly different spatiotemporal features compared to Newtonian turbulence, termed elastoinertial turbulence (EI...

We perform simulations of an impulsively-started, axisymmetric viscoelastic jet exiting a nozzle and entering a stagnant gas phase using the open-source code Basilisk. This code allows for efficient computations through an adaptively-refined volume-of-fluid technique that can accurately capture the deformation of the liquid-gas interface. We use th...

The rod-climbing or “Weissenberg” effect, in which the free surface of a complex fluid climbs a thin rotating rod, is a popular and convincing experiment demonstrating the existence of elasticity...

The superposition of data sets with internal parametric self-similarity is a longstanding and widespread technique for the analysis of many types of experimental data across the physical sciences. Typically, this superposition is performed manually, or recently through the application of one of a few automated algorithms. However, these methods are...

Soft particulate gels are composed of a small amount of particulate matter dispersed in a continuous fluid phase. The solid components assemble to form a porous matrix, providing rigidity and control of the mechanical response, despite being the minority constituent. The rheological response and gel elasticity are direct functions of the particle v...

Addition of particles to a viscoelastic suspension dramatically alters the properties of the mixture, particularly when it is sheared or otherwise processed. Shear-induced stretching of the polymers results in elastic stress that causes a substantial increase in measured viscosity with increasing shear, and an attractive interaction between particl...

A laser pulse focused near the closed end of a glass capillary partially filled with water creates a vapor bubble and an associated pressure wave. The pressure wave travels through the liquid toward the meniscus where it is reflected, creating a fast, focused microjet. In this study, we selectively coat the hydrophilic glass capillaries with hydrop...

Oscillatory rheometric techniques such as small amplitude oscillatory shear (SAOS) and, more recently, medium amplitude oscillatory shear and large amplitude oscillatory shear (LAOS) are widely used for rheological characterization of the viscoelastic properties of complex fluids. However, in a time-evolving or mutating material, the build-up or br...

Micro-prosthetics requires the fabrication of mechanically robust and personalized components with sub-millimetric feature accuracy. Three-dimensional (3D) printing technologies have had a major impact on manufacturing such miniaturized devices for biomedical applications; however, biocompatibility requirements greatly constrain the choice of usabl...

Solutions of polymer chains are modelled using non-equilibrium Brownian dynamics simulations, with physically associative beads which form reversible crosslinks to establish a system-spanning physical gel network. Rheological properties such as zero-shear viscosity and relaxation modulus are investigated systematically as functions of polymer conce...

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 ext...

A laser pulse focused near the closed end of a glass capillary partially filled with water creates a vapor bubble and an associated pressure wave. The pressure wave travels through the liquid toward the meniscus where it is reflected, creating a fast, focused microjet. In this study, we selectively coat the hydrophilic glass capillaries with hydrop...

This study examines the movement of a small freely rotating spherical particle in a two-dimensional trajectory through a viscoelastic fluid described by the Giesekus model. The fluid equations of motion in the inertialess limit and the Giesekus constitutive equation are expanded as a power series in the Weissenberg number, for which analytical solu...

Viscoelastic stress relaxation is a basic characteristic of soft matter systems such as colloids, gels, and biological net-works. Although the Maxwell model of linear viscoelasticity provides a classical description of stress relaxation, the Maxwell model is often not sufficient for capturing the complex relaxation dynamics of soft matter. In this...

Soft particulate gels include materials we can eat, squeeze, or 3D print. From foods to bio-inks to cement hydrates, these gels are composed of a small amount of particulate matter (proteins, polymers, colloidal particles, or agglomerates of various origins) embedded in a continuous fluid phase. The solid components assemble to form a porous matrix...

We provide a canonical introduction to dual-junction-functionality associative polymer networks, which combine high and low functionality ( f) dynamic cross-link junctions to impart load-bearing, dissipation, and self-repairing ability to the network. This unique type of network configuration offers an alternative to traditional dual-junction netwo...

The FENE-P (Finitely-Extensible Nonlinear Elastic) dumbbell constitutive equation is widely used in simulations and stability analyses of free and wall-bounded viscoelastic shear flows due to its relative simplicity and accuracy in predicting macroscopic properties of dilute polymer solutions. The model contains three independent material parameter...

Aqueous foams are useful in several applications, especially to reduce liquid loading in the oil and gas industry. The rheology of these foams evolves rapidly, and suitable constitutive models are required to describe the resulting multiphase flow. We describe a new experimental setup for advanced rheometry involving 4-arm and 12-arm vane-in-textur...

The formulation of rheological constitutive equations -- models that relate internal stresses and deformations in complex fluids -- is a critical step in the engineering of systems involving soft materials. While data-driven models provide accessible alternatives to expensive first-principles models and less accurate empirical models in many engine...

Nanocomposites formed by mixing nanoparticles and polymers offer a limitless creative space for the design of functional advanced materials with a broad range of applications in materials and biological sciences. Here we focus on aqueous dispersions of hydrophobic colloidal soot particles, namely carbon black (CB) dispersed with a sodium salt of ca...

The concept of a Deborah number is widely used in the study of viscoelastic materials to represent the ratio of a material relaxation time to the time scale of observation and to demarcate transitions between predominantly viscous or elastic material responses. However, this construct does not help quantify the importance of long transients and non...

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 surpri...

The FENE-P (Finitely-Extensible Nonlinear Elastic) dumbbell constitutive equation is widely used in simulations and stability analyses of free and wall-bounded viscoelastic shear flows due to its relative simplicity and accuracy in predicting macroscopic properties of dilute polymer solutions. The model contains three independent material parameter...

Carbonated droplets deposited on a superhydrophobic surface float on a self-generated cushion of gas.

Arrested soft materials such as gels and glasses exhibit a slow stress relaxation with a broad distribution of relaxation times in response to linear mechanical perturbations. Although this macroscopic stress relaxation is an essential feature in the application of arrested systems as structural materials, consumer products, foods, and biological m...

The interplay between viscoelasticity and inertia in dilute polymer solutions at high deformation rates can result in inertio-elastic instabilities. The nonlinear evolution of these instabilities generates a state of turbulence with significantly different spatio-temporal features compared to Newtonian turbulence, termed elasto-inertial turbulence...

Shear thickening denotes the reversible increase in viscosity of a suspension of rigid particles under external shear. This ubiquitous phenomenon has been documented in a broad variety of multiphase particulate systems, while its microscopic origin has been successively attributed to hydrodynamic interactions and frictional contact between particle...

A number of commercial fluids, including synthetic automotive oils, food and consumer products containing polymer additives exhibit weakly rate-thickening responses in the final stages of capillarity-driven thinning, where a large accumulated strain and high extensional strain rate alter the thinning dynamics of the slender liquid filament. Consequ...

We analyze the capillarity-driven thinning dynamics of entangled polymer solutions described by the Doi-Edwards-Marrucci-Grizzuti (DEMG) model and the Rolie-Poly (RP) model. Both models capture polymer reptation, finite rates of chain retraction and finite extensibility of single polymer molecules, while differing slightly in their final form regar...

A planar two-dimensional computational analysis is presented to qualify traditional and fractal vane-in-cup geometries for accurate rheometry of simple viscoplastic fluids with and without slip. Numerical simulations based on an adaptive augmented Lagrangian scheme are used to study the two-dimensional flow field of yield-stress fluids within and a...

Chlorosulfonic acid and oleum are ideal solvents for enabling the transformation of disordered carbon nanotubes (CNTs) into precise and highly functional morphologies. Currently, processing these solvents using extrusion techniques presents complications due to chemical compatibility, which constrain equipment and substrate material options. Here,...

The superposition of data sets with internal parametric self-similarity is a longstanding and widespread technique for the analysis of many types of experimental data across the physical sciences. Typically, this superposition is performed manually, or recently by one of a few automated algorithms. However, these methods are often heuristic in natu...

The mechanical experience of consumption (i.e., feel, softness, and texture) of many foods is intrinsic to their enjoyable consumption, one example being the habit of twisting a sandwich cookie to reveal the cream. Scientifically, sandwich cookies present a paradigmatic model of parallel plate rheometry in which a fluid sample, the cream, is held b...

Accurately resolving the coupled momentum transfer between the liquid and solid phases of complex fluids is a fundamental problem in multiphase transport processes, such as hydraulic fracture operations. Specifically we need to characterize the dependence of the normalized average fluid–particle force ⟨F⟩\documentclass[12pt]{minimal} \usepackage{am...

In this work, we mathematically derive the conditions for which empirical rheometric relations such as the Cox–Merz rule and Gleissle mirror relationship are satisfied. We consider the Wagner integral constitutive framework, which is a special limiting case of the Kaye–Bernstein Kearsley Zapas (K-BKZ) constitutive equation to derive analytical expr...