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DOE OSTI2024

Solvent-Dependent Dynamics of Cellulose Nanocrystals in Process-Relevant Flow Fields

Flow-assisted alignment of anisotropic nanoparticles is a promising route for the bottom-up assembly of advanced materials with tunable properties. While aligning processes could be optimized by controlling factors such as solvent viscosity, flow deformation, and the structure of the particles themselves, it is necessary to understand the relationship between these factors and their effect on the final orientation. In this study, we investigated the flow of surface-charged cellulose nanocrystals (CNCs) with the shape of a rigid rod dispersed in water and propylene glycol (PG) in an isotropic tactoid state. In situ scanning small-angle X-ray scattering (SAXS) and rheo-optical flow-stop experiments were used to quantify the dynamics, orientation, and structure of the assigned system at the nanometer scale. The effects of both shear and extensional flow fields were revealed in a single experiment by using a flow-focusing channel geometry, which was used as a model flow for nanomaterial assembly. Due to the higher solvent viscosity, CNCs in PG showed much slower Brownian dynamics than CNCs in water and thus could be aligned at lower deformation rates. Moreover, CNCs in PG also formed a characteristic tactoid structure but with less ordering than CNCs in water owing to weaker electrostatic interactions. The results indicate that CNCs in water stay assembled in the mesoscale structure at moderate deformation rates but are broken up at higher flow rates, enhancing rotary diffusion and leading to lower overall alignment. Albeit being a study of cellulose nanoparticles, the fundamental interplay between imposed flow fields, Brownian motion, and electrostatic interactions likely apply to many other anisotropic colloidal systems.

36 MATERIALS SCIENCE↗

NASA NTRS1999

Computations of Boiling in Microgravity

Tryggvason, Gretar↗

NASA NTRS2000

Computations of Boiling in Microgravity

The absence (or reduction) of gravity, can lead to major changes in boiling heat transfer. On Earth, convection has a major effect on the heat distribution ahead of an evaporation front, and buoyancy determines the motion of the growing bubbles. In microgravity, convection and buoyancy are absent or greatly reduced and the dynamics of the growing vapor bubbles can change in a fundamental way. In particular, the lack of redistribution of heat can lead to a large superheat and explosive growth of bubbles once they form. While considerable efforts have been devoted to examining boiling experimentally, including the effect of microgravity, theoretical and computational work have been limited. Here, the growth of boiling bubbles is studied by direct numerical simulations where the flow field is fully resolved and the effects of inertia, viscosity, surface deformation, heat conduction and convection, as well as the phase change, are fully accounted for. Boiling involves both fluid flow and heat transfer and thus requires the solution of the Navier-Stokes and the energy equations. The numerical method is based on writing one set of governing transport equations which is valid in both the liquid and vapor phases. This local, single-field formulation incorporates the effect of the interface in the governing equations as source terms acting only at the interface. These sources account for surface tension and latent heat in the equations for conservation of momentum and energy as well as mass transfer across the interface due to phase change. The single-field formulation naturally incorporates the correct mass, momentum and energy balances across the interface. Integration of the conservation equations across the interface directly yields the jump conditions derived in the local instant formulation for two-phase systems. In the numerical implementation, the conservation equations for the whole computational domain (both vapor and liquid) are solved using a stationary grid and the phase boundary is followed by a moving unstructured two-dimensional grid. While two-dimensional simulations have been used for preliminary studies and to examine the resolution requirement, the focus is on fully three-dimensional simulations. The numerical methodology, including the parallelization and grid refinement strategy is discussed, and preliminary results shown. For buoyancy driven flow, the heat transfer is in good agreement with experimental correlations. The changes when gravity is turned off and/or fluid shear is added are discussed, as well as the difference between simulations of a layer freely releasing bubbles versus simulations using only one wavelength initial perturbation. Figure 1 shows the early stages of the formation of a three-dimensional bubble from a thin vapor layer. The boundary conditions are periodic in the x and y direction, the bottom is a hot and the top allows a free outflow. The jagged edge of the surface close to the bottom of the computational domain is due to some of the surface elements being on the other side of the domain and some elements not plotted by our plotting routine. In the second figure, we show the temperature distribution through two perpendicular planes.

Tryggvason, G.↗

NASA NTRS1994

Control of cytoskeletal mechanics by extracellular matrix, cell shape, and mechanical tension

We have investigated how extracellular matrix (ECM) alters the mechanical properties of the cytoskeleton (CSK). Mechanical stresses were applied to integrin receptors on the apical surfaces of adherent endothelial cells using RGD-coated ferromagnetic microbeads (5.5-microns diameter) in conjunction with a magnetic twisting device. Increasing the number of basal cell-ECM contacts by raising the fibronectin (FN) coating density from 10 to 500 ng/cm2 promoted cell spreading by fivefold and increased CSK stiffness, apparent viscosity, and permanent deformation all by more than twofold, as measured in response to maximal stress (40 dyne/cm2). When the applied stress was increased from 7 to 40 dyne/cm2, the stiffness and apparent viscosity of the CSK increased in parallel, although cell shape, ECM contacts, nor permanent deformation was altered. Application of the same stresses over a lower number ECM contacts using smaller beads (1.4-microns diameter) resulted in decreased CSK stiffness and apparent viscosity, confirming that this technique probes into the depth of the CSK and not just the cortical membrane. When magnetic measurements were carried out using cells whose membranes were disrupted and ATP stores depleted using saponin, CSK stiffness and apparent viscosity were found to rise by approximately 20%, whereas permanent deformation decreased by more than half. Addition of ATP (250 microM) under conditions that promote CSK tension generation in membrane-permeabilized cells resulted in decreases in CSK stiffness and apparent viscosity that could be detected within 2 min after ATP addition, before any measurable change in cell size.(ABSTRACT TRUNCATED AT 250 WORDS).

Non-NASA Center↗

DOE OSTI2025

Topology-Dependent Polymer Stretching and Scission in Solution at Extreme Shear Rates

There has been significant interest in the engineering of polymer topology to control rheology and mechanical stability in dilute solutions for applications involving extreme shear rate flows. However, methods to experimentally probe properties at relevant shear rates (≈ 10 4 –10 6 s –1 ) have remained ex situ, obscuring access to measures of polymer deformation and rheology that would otherwise provide mechanistic insight into the topology-dependent properties that control their behavior in extreme shear flows. In this study, we used novel in situ small angle neutron scattering measurements in a capillary rheometer (capillary rheo-SANS) to simultaneously measure solution viscosities and polymer deformations in high shear on a series of chemically homologous topology-defined polymers including linear, randomly branched, and star-shaped molecules. We demonstrate that differences in the onset of chain stretching and shear thinning of these polymers in dilute solution are controlled primarily by differences in their molecular relaxation time. These differences correlate with differences in chain scission inferred from ex situ measurements at more extreme shear rates. Together, the results demonstrate a direct coupling between chain deformation and scission, and suggest that the dominant effect of branching as a means to impart resilience against mechanical degradation is through differences in relaxation dynamics due to branching. We anticipate that these results will provide key insights to engineer topology-controlled polymers for rheological modification, mechanical stability, and controlled mechano-chemistry.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

NASA NTRS1994

Modeling of periodic great earthquakes on the San Andreas fault: Effects of nonlinear crustal rheology

We analyze the cycle of great earthquakes along the San Andreas fault with a finite element numerical model of deformation in a crust with a nonlinear viscoelastic rheology. The viscous component of deformation has an effective viscosity that depends exponentially on the inverse absolute temperature and nonlinearity on the shear stress; the elastic deformation is linear. Crustal thickness and temperature are constrained by seismic and heat flow data for California. The models are for anti plane strain in a 25-km-thick crustal layer having a very long, vertical strike-slip fault; the crustal block extends 250 km to either side of the fault. During the earthquake cycle that lasts 160 years, a constant plate velocity v(sub p)/2 = 17.5 mm yr is applied to the base of the crust and to the vertical end of the crustal block 250 km away from the fault. The upper half of the fault is locked during the interseismic period, while its lower half slips at the constant plate velocity. The locked part of the fault is moved abruptly 2.8 m every 160 years to simulate great earthquakes. The results are sensitive to crustal rheology. Models with quartzite-like rheology display profound transient stages in the velocity, displacement, and stress fields. The predicted transient zone extends about 3-4 times the crustal thickness on each side of the fault, significantly wider than the zone of deformation in elastic models. Models with diabase-like rheology behave similarly to elastic models and exhibit no transient stages. The model predictions are compared with geodetic observations of fault-parallel velocities in northern and central California and local rates of shear strain along the San Andreas fault. The observations are best fit by models which are 10-100 times less viscous than a quartzite-like rheology. Since the lower crust in California is composed of intermediate to mafic rocks, the present result suggests that the in situ viscosity of the crustal rock is orders of magnitude less the rock viscosity determined in the laboratory.

Reches, Ze'ev↗

DOE OSTI2025

In situ deformation of antigorite-olivine two-phase mixtures: Implications for dynamics and seismic anisotropy in the mantle wedge

Water released from hydrous minerals in subducting slabs reacts with the overlying plate, resulting in widespread serpentinization in the mantle wedge. Deformation of serpentinized peridotites has been invoked to explain forearc seismic anisotropy, yet studies of the mechanical properties and deformation behaviors of serpentine-bearing multiphase aggregates remain limited. Here we deformed olivine-antigorite mixtures containing 70, 50, and 20 vol.% of antigorite at 2.5 – 7.6 GPa, 673 K and strain rates of ∼10 –5 –10 –4 s –1 . Elasto-viscoplastic self-consistent simulations, constrained by synchrotron X-ray diffraction (XRD) data, were used to estimate lattice strain, stress–strain partitioning, crystallographic preferred orientations (CPO) development, and aggregate strength. Selected run products were also analyzed by electron backscatter diffraction for comparison with the CPO results obtained from XRD experiments. We found olivine transitions from A- or B-type to C-type when antigorite fraction drops to 20 vol.%, coinciding with a microstructural change from interconnected weak layers to a load-bearing framework (LBF). An additional run on a sample Atg50/Ol50 with preexisting microstructures suggested the formation of LBF was promoted by these microstructures, although the preexisting antigorite CPO has been overprinted at 20.8 % strain and could be erased completely by subsequent deformation in nature. Estimated viscosity of the two-phase mixtures suggests that low-degree serpentinization (≤20 %) in the mantle wedge may increase the strength of olivine-rich peridotite and hinder slab-mantle decoupling, whereas high-degree serpentinization (≥50–70 %) weakens the peridotite and favors decoupling if sufficient viscosity contrast (>10) develops. Seismic anisotropy shows a nonlinear dependence on antigorite fraction: antigorite CPO governs the anisotropy of the mixtures with ≥50 vol.% antigorite, whereas olivine CPO dominates at low fractions (∼20 vol.%). The presence of pre-existing microstructures reduces seismic anisotropy of the deformed mixtures, however the persistence of pre-existing CPO in actively subducting slabs remains uncertain, making their significance over geological timescales questionable.

Crystallographic preferred orientation↗

NASA NTRS1994

Viscosity estimates for the crust and upper mantle from patterns of lacustrine shoreline deformation in the Eastern Great Basin

The deformed shorelines of Lake Bonneville constitute a classic source of information on lithospheric elastic thickness and upper mantle viscosity. We describe and apply a new model to a recently augmented data set. New data better constrain both the complex spatio-temporal pattern of the lake load and the crustal deformation response to that load. The history of lake level fluctuations has been significantly refined and somewhat modified. This is due to both more radiocarbon dates from within the Bonneville basin and to an improved calibration of the radiocarbon timescale itself. The data which constrain the crustal deformation pattern consist of ages and shoreline elevations from several hundred points which sample three major levels of Lake Bonneville and corresponding elevations from the high stands of three smaller lakes situated to the west of Lake Bonneville. The geometry of the Earth model incorporates an arbitrary number of layers overlying a half-space, and the rheology of each level can accommodate an arbitrary number of Maxwell viscoelastic elements in parallel. The inverse modeling comprises three complementary approaches: for the simplest configurations, we performed a direct search of the parameter space and delineated the irregular boundary of the subspace of acceptable models. For more complex configurations, we constrained the elastic parameters to their seismically determined values and then solved for viscosity versus depth profiles by either expressing the log(viscosity) versus log(depth) profile as a series of specially constructed orhtogonal polynomials, or by allowing each of 8-10 layers (plus the half-space) to have an independently determined viscosity. We found that the data do not strongly support (nor can they conclusively exclude) a more complex rheology than simple Maxwell viscoelasticity. The orthogonal polynomial solution exhibits an essentially monotonic decrease in viscosity with depth.

Bills, Bruce G.↗

DOE OSTI2023

World beyond the nearest neighbors

The structure beyond the nearest neighbor atoms in liquid and glass is characterized by the medium-range order (MRO). In the conventional approach, the MRO is considered to result directly from the short-range order (SRO) in the nearest neighbors. To this bottom–up approach starting with the SRO, we propose to add a top–down approach in which global collective forces drive liquid to form density waves. The two approaches are in conflict with each other, and the compromise produces the structure with the MRO. The driving force to produce density waves provides the stability and stiffness to the MRO, and controls various mechanical properties. This dual framework provides a novel perspective for description of the structure and dynamics of liquid and glass.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Medium-Range Order Resists Deformation in Metallic Liquids and Glasses

In crystals, lattice defects, such as dislocations, control mechanical deformation. Similarly, it is widely believed that even in glasses and liquids some kinds of defects, strongly disordered regions, play a major role in deformation. To identify defects researchers focused on the nature of the short-range order (SRO) in the nearest neighbor cage of atoms. However, recent results by experiment, simulation and theory raise serious questions about this assumption. They suggest that the atomic medium-range order (MRO) provides resistance against flow at the atomic level. Because the MRO is a bulk property, it implies that defects play only a limited role. This new insight is supported by the density wave theory which shows that the MRO is driven by a top-down global force, rather than being a consequence of the SRO in the bottom-up manner, and the MRO provides stiffness to resist deformation. We briefly summarize the density wave theory, show that the MRO is related to ductility of metallic glasses, and discuss the implications on the role of the MRO in the atomic-level mechanism of deformation.

36 MATERIALS SCIENCE↗

NASA NTRS1980

Equilibrium geochemical modeling of a seasonal thermal energy storage aquifer field test

A geochemical mathematical modeling study designed to investigate the well plugging problems encountered at the Auburn University experimental field tests is summarized. The results, primarily of qualitative interest, include: (1) loss of injectivity was probably due to a combination of native particulate plugging and clay swelling and dispersion; (2) fluid-fluid incompatibilities, hydrothermal reactions, and oxidation reactions were of insignificant magnitude or too slow to have contributed markedly to the plugging; and (3) the potential for and contributions from temperature-induced dissolved gas solubility reductions, capillary boundary layer viscosity increases, and microstructural deformation cannot be deconvolved from the available data.

Stottlemyre, J. S.↗

NASA NTRS1980

Time dependent deformation and stress in the lithosphere

Efficient computer programs incorporating frontal solution and time stepping procedure were developed for the modelling of geodynamic problems. This scheme allows for investigating the quasi static phenomena including the effects of the rheological structure of a tectonically active region. From three dimensional models of strike slip earthquakes, it was found that lateral variation of viscosity affects the characteristics of surface deformations. The vertical deformation is especially informative about the viscosity structure in a strike slip fault zone. A three dimensional viscoelastic model of a thrust earthquake indicated that the transient disturbance on plate velocity due to a great plate boundary earthquake is significant at intermediate distances, but becomes barely measurable 1000 km away from the source.

Yang, M.↗

NASA NTRS1980

Extensional flow of dilute polymer solution

Simultaneous effects of temperature and concentration on tensile viscosity are investigated using a semi-empirical scaling law established to relate the concentration, temperature and deformation rate by a reduced deformation rate variable. Results show the onset of high viscosity occurring in the vicinity of the onset of non-Newtonian viscosity observed in a simple shear flow experiment. High viscosity is also compared with steady and dynamic shear data. Finally, the asymptotic solution of Hassager's kinetic theory of a bead-rod model for macromolecular solutions is compared with the data, indicating that tensile viscosity depends strongly on the molecular weight, the higher the molecular weight, the more sensitive the tensile viscosity in terms of the deformation rate.

Peng, S. T. J.↗

DOE OSTI2025

Multipolar Fermi Surface Deformations in Sr 2 ⁢RuO 4 Probed by Resistivity and Sound Attenuation: A Window into Electron Viscosity and the Collision Operator

Recent developments in electron hydrodynamics have demonstrated the importance of considering the full structure of the electron-electron scattering operator, which encodes a sequence of lifetimes, one for each component of the Fermi surface deformation in a multipolar expansion. In this context, the dipolar lifetime is measured by resistivity, whereas the quadrupolar component probes the viscosity and can be measured in the bulk via sound attenuation. We introduce a framework to extract the collision operator of an arbitrary metal by combining resistivity and sound attenuation measurements with a realistic calculation of the scattering operator that includes multiband and umklapp effects. The collision operator allows for the prediction of a plethora of properties, including the nonlocal conductivity, and can be used to predict hydrodynamic behavior for bulk metals. As a first application, we apply this framework to Sr 2 ⁢RuO 4 in a temperature range where electron-electron scattering is dominant. Furthermore, we find quantitative agreement between our model and the temperature dependence of both the resistivity and the sound attenuation, we find the quadrupolar (𝐵 1⁢𝑔 ) relaxation rate to be 30% higher than the dipolar one due to the presence of hot spots on the 𝛾 band, and we predict a strongly anisotropic viscosity arising from the 𝛼 and 𝛽 bands.

Boltzmann theory↗

NASA NTRS1975

Recent and late quaternary changes in water level

Water level changes of both the Great Lakes and the sea are described along with methods of analyzing water level data. The influence of elastic deformation of the earth and viscosity is discussed. Causes of water level changes reviewed include: earth movements, geoid changes, storm surges or meteorological phenomena, and melting ice in Antarctica, Greenland, and the mountain glaciers.

R. I. Walcott↗

NASA NTRS2000

Reduction of Effective Acceleration to Microgravity Levels

Acceleration due to earth's gravity causes buoyancy driven convection and sedimentation in solutions. In addition. pressure gradients occur as a function of the height within a liquid column. Hence gravity effects both equilbria conditions and phase transitions as a result of hydrostatic pressure gradients. The affect of gravity on the rate of heat and man transfer in solutal processes can be particularly important in polymer processing due to the high sensitivity of polymeric materials to processing conditions. The term microgravity has been coined to describe an environment in which the affects of gravitational acceleration am greatly reduced. It may seem odd to talk in term of reducing the effects of gravitational acceleration since gravitational attraction is a basic property of matter. However, die presence of gravity on in situ processing or measurements can be negated by achieving conditions in which the laboratory, or more specifically the container of the experimental materials, a subjected to the same acceleration as the materials themselves. With regard to the laboratory reference frame, there is virtually no force on the experimental solutions. This is difficult to achieve but can be done. A short review of Newtonian physics provides an explanation on both how processes we affected by gravity and how microgravity conditions are achieved. The fact that fluids deform when subject to a force bid solids do not indicates that solids have a structure able to exert an opposing force that negates an externally applied force. Liquids deform when a force is applied, indicating that a liquid structure cannot completely negate an applied force. Just how easily a liquid resists deformation is related to its viscosity. Spaceflight provides an environment in which the laboratory reference frame i.e. the spacecraft and all the equipment therein an experiencing virtually identical forces. There is no solid foundation underneath such a laboratory, so the laboratory accelerates according to the force of gravity as do the experimental fluids within the lab. Hence, the magnitude of the form excited by the laboratory on the experimental solutions within are greatly reduced. When compared with a laboratory on the ground and averaged over time, the fluids in a spaceflight laboratory experience approximately a 10 (sup -6)decrease in acceleration relative to their laboratory reference frame hence the term microgravity.

Downey, James P.↗

NASA NTRS2002

Laminar-Turbulent Transition in an Electromagnetically-Levitated Droplet

During experiments on the MSL-1 (First Microgravity Science Laboratory) mission of the Space Shuttle (STS-83 and STS-94, April and July 1997), a droplet of palladium-silicon alloy was electromagnetically levitated for viscosity measurements. For the non-deforming droplet, the resultant MHD flow inside the drop can be inferred from motion of impurity particulates on the surface. In the experiments, subsequent to melting, Joule heating produces a continuous reduction of viscosity of the fluid resulting in an acceleration of the flow with time. These observations indicate formation of a pair of co-rotating toroidal flow structures inside the spheroidal drop that undergo flow instabilities. As the fluid temperature rises, the amplitude of the secondary flow increases; and beyond a point, the tracers exhibit non-coherent chaotic motion signifying emergence of turbulence inside the drop. Assuming that the observed laminar-turbulent transition is shear-layer type, the internal structure of the toroidal loops is used to develop a semi- empirical correlation for the onset of turbulence. Our calculations indicate that the suggested correlation is in modest agreement with the experimental data, with the transition occurring at a Reynolds number of 600.

Hyers, R. W.↗

NASA NTRS2002

Laminar-Turbulent Transition in an Electromagnetically-Levitated Droplet

During experiments on the MSL-1 (First Microgravity Science Laboratory) mission of the Space Shuttle (STS-83 and STS-94, April and July 1997), a droplet of palladium-silicon alloy was electromagnetically levitated for viscosity measurements. For the non-deforming droplet, the resultant MHD flow inside the drop can be inferred from motion of impurity particulates on the surface. In the experiments, subsequent to melting, Joule heating produces a continuous reduction of viscosity of the fluid resulting in an acceleration of the flow with time. These observations indicate formation of a pair of corotating toroidal flow structures inside the spheroidal drop that undergo flow instabilities. As the fluid temperature rises, the amplitude of the secondary flow increases; and beyond a point, the tracers exhibit non-coherent chaotic motion signifying emergence of turbulence inside the drop. Assuming that the observed laminar-turbulent transition is shear-layer type, the internal structure of the toroidal loops is used to develop a semi-empirical correlation for the onset of turbulence. Our calculations indicate that the suggested correlation is in modest agreement with the experimental data, with the transition occurring at a Reynolds number of 600.

Hyers, Robert W.↗