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McKinley, Gareth H.

Publications and source records attributed to McKinley, Gareth H..

Aluminosilicate colloidal gels: from the early age to the precipitation of zeolites

Aluminosilicate hydrogels are often considered to be precursors for the crystallisation of zeolites carried out under hydrothermal conditions. The preparation of mechanically homogeneous aluminosilicate gels enables the study of these materials through bulk rheology and observation of the aging dynamics until the precipitation of crystalline zeolites. The first part of this study deals with the establishment of ternary state diagrams, in order to identify the range of chemical formulations that enable preparation of single-phase homogeneous gels. Then, by studying the viscoelastic moduli during the gelation reaction, and by yielding the gel under large deformation, we propose an empirical law considering the partial order of reaction on each chemical element, to predict the gelation time according to the chemical formulation. The scaling behavior of the elastic properties of this colloidal gel shows a transition from a strong link behavior to a weak link regime. Long term aging results in the shrinkage of the gel, accompanied by syneresis of interstitial liquid at the surface. Zeolites precipitate through crystallisation by a particle attachment mechanism, when thermodynamic equilibrium is reached. The stoichiometry of the precipitated zeolites is not only consistent with the concentration of the remaining species in the supernatant but, surprisingly, it is also very close to the partial order of the reaction of the chemical elements involved in the determination of the critical gel point. This indicates a strong correlation between the morphology of the soft amorphous gel network that is formed at an early age and those of the final solid precipitated crystals.

36 MATERIALS SCIENCE↗

Scientific machine learning for modeling and simulating complex fluids

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 disciplines, the development of similar models for complex fluids has lagged. The diversity of techniques for characterizing non-Newtonian fluid dynamics creates a challenge for classical machine learning approaches, which require uniformly structured training data. Consequently, early machine-learning based constitutive equations have not been portable between different deformation protocols or mechanical observables. Here, we present a data-driven framework that resolves such issues, allowing rheologists to construct learnable models that incorporate essential physical information, while remaining agnostic to details regarding particular experimental protocols or flow kinematics. These scientific machine learning models incorporate a universal approximator within a materially objective tensorial constitutive framework. By construction, these models respect physical constraints, such as frame-invariance and tensor symmetry, required by continuum mechanics. We demonstrate that this framework facilitates the rapid discovery of accurate constitutive equations from limited data and that the learned models may be used to describe more kinematically complex flows. This inherent flexibility admits the application of these “digital fluid twins” to a range of material systems and engineering problems. We illustrate this flexibility by deploying a trained model within a multidimensional computational fluid dynamics simulation—a task that is not achievable using any previously developed data-driven rheological equation of state.

Science & Technology - Other Topics↗

Preliminary Findings from the SHERE ISS Experiment

The Shear History Extensional Rheology Experiment (SHERE) is an International Space Station (ISS) glovebox experiment designed to study the effect of preshear on the transient evolution of the microstructure and viscoelastic tensile stresses for monodisperse dilute polymer solutions. The SHERE experiment hardware was launched on Shuttle Mission STS-120 (ISS Flight 10A) on October 22, 2007, and 20 fluid samples were launched on Shuttle Mission STS-123 (ISS Flight 10/A) on March 11, 2008. Astronaut Gregory Chamitoff performed experiments during Increment 17 on the ISS between June and September 2008. A summary of the ten year history of the hardware development, the experiment's science objectives, and Increment 17's flight operations are discussed in the paper. A brief summary of the preliminary science results is also discussed.

Hall, Nancy R.↗

The Considere Condition and Rapid Stretching of Linear and Branched Polymer Melts

We analyze the onset of "necking" and subsequent filament failure during the transient uniaxial elongation of viscoelastic fluid samples in extensional rheometers. In the limit of rapid elongation (such that no molecular relaxation occurs), the external work applied is all stored elastically and the Considere criterion originally developed in solid mechanics can be used to quantitatively predict the critical Hencky strain to failure. By comparing the predictions of the Doi-Edwards model for linear homopolymer melts with those of the "Pom-Pom" model for prototypical branched melts we show that the critical strain to failure in rapid elongation of a rubbery material is intimately linked to the molecular topology of the chain, especially the degree of chain branching. The onset of necking instability is monotonically shifted to larger Hencky strains as the number of branches is increased. Numerical computations at finite Deborah numbers also show that there is an optimal range of deformation rates over which homogeneous extensions can be maintained to large strain. We also consider other rapid homogeneous stretching deformations, such as biaxial and planar stretching, and show that the degree of stabilization afforded by inclusion of material with long-chain branching is a sensitive function of the imposed mode of deformation.

McKinley, Gareth H.↗

Extensional Flow of a Polystyrene Boger Fluid Through a 4:1:4 Axisymmetric Contraction/Expansion

The creeping flow of a dilute (0.025 wt%) monodisperse polystyrene/polystyrene Boger fluid through a 4:1:4 axisymmetric contraction/expansion is experimentally observed for a wide range of Deborah numbers. Pressure drop measurements across the orifice plate show a large extra pressure drop that increases monotonically with Deborah number above the value observed for a similar Newtonian fluid at the same flow rate. This enhancement in the dimensionless pressure drop is not associated with the onset of a flow instability, yet it is not predicted by existing steady-state or transient numerical computations with simple dumbbell models. It is conjectured that this extra pressure drop is the result of an additional dissipative contribution to the polymeric stress arising from a stress-conformation hysteresis in the strong non-homogeneous extensional flow near the contraction plane. Such a hysteresis has been independently measured and computed in recent studies of homogeneous transient uniaxial stretching of PS/PS Boger fluids. Flow visualization and velocity field measurements using digital particle image velocimetry (DPIV) show large upstream growth of the corner vortex with increasing Deborah number. At large Deborah numbers, the onset of an elastic instability is observed, first locally as small amplitude fluctuations in the pressure measurements, and then globally as an azimuthal precessing of the upstream corner vortex accompanied by periodic oscillations in the pressure drop across the orifice.

Rothstein, Jonathan P.↗

A Compact Dual-Crystal Modulated Birefringence-Measurement System for Microgravity Applications

A compact modulated birefringence-measurement system has been developed for use in microgravity fluid physics applications with non-Newtonian fluids such as polymer solutions. This instrument uses a dual-crystal transverse electro-optical modulator capable of modulation frequencies in excess of 100 MHz. The two crystals are modulated 180 deg. out of phase from each other, The theoretical framework governing the development of this instrument using the Mueller-Stokes polarization matrices is discussed. Several ground-based experiments are performed to compare this system with the theoretical results. Results from this transverse electro-optical modulator-based birefringence-measurement system agree well with the theory. The instrument is also very stable and robust, making it suitable for the extreme acceleration environment to be encountered in a NASA Black Brandt sounding rocket.

Mackey, Jeffrey R.↗

The Extensional Rheology of Non-Newtonian Materials

The evolution of the transient extensional stresses in dilute and semi-dilute viscoelastic polymer solutions are measured with a filament stretching rheometer of a design similar to that first introduced by Sridhar, et al. The solutions are polystyrene-based (PS) Boger fluids that are stretched at constant strain rates ranging from 0.6 less than or equal to epsilon(0) less than or equal to 4s(exp -1) and to Hencky strains of epsilon greater than 4. The test fluids all strain harden and Trouton ratios exceeding 1000 are obtained at high strains. The experimental data strain hardens at lower strain levels than predicted by bead-spring FENE models. In addition to measuring the transient tensile stress growth, we also monitor the decay of the tensile viscoelastic stress difference in the fluid column following cessation of uniaxial elongation as a function of the total imposed Hencky strain and the strain rate. The extensional stresses initially decay very rapidly upon cessation of uniaxial elongation followed by a slower viscoelastic relaxation, and deviate significantly from FENE relaxation predictions. The relaxation at long times t is greater than or equal to 5 s, is compromised by gravitational draining leading to non-uniform filament profiles. For the most elastic fluids, partial decohension of the fluid filament from the endplates of the rheometer is observed in tests conducted at high strain rates. This elastic instability is initiated near the rigid endplate fixtures of the device and it results in the progressive breakup of the fluid column into individual threads or 'fibrils' with a regular azimuthal spacing. These fibrils elongate and bifurcate as the fluid sample is elongated further. Flow visualization experiments using a modified stretching device show that the instability develops as a consequence of an axisymmetry-breaking meniscus instability in the nonhomogeneous region of highly deformed fluid near the rigid endplate.

Spiegelberg, Stephen H.↗