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DOE OSTI2024

De novo design of modular protein hydrogels with programmable intra- and extracellular viscoelasticity

Relating the macroscopic properties of protein-based materials to their underlying component microstructure is an outstanding challenge. Here, we exploit computational design to specify the size, flexibility, and valency of de novo protein building blocks, as well as the interaction dynamics between them, to investigate how molecular parameters govern the macroscopic viscoelasticity of the resultant protein hydrogels. We construct gel systems from pairs of symmetric protein homo-oligomers, each comprising 2, 5, 24, or 120 individual protein components, that are crosslinked either physically or covalently into idealized step-growth biopolymer networks. Through rheological assessment, we find that the covalent linkage of multifunctional precursors yields hydrogels whose viscoelasticity depends on the crosslink length between the constituent building blocks. In contrast, reversibly crosslinking the homo-oligomeric components with a computationally designed heterodimer results in viscoelastic biomaterials exhibiting fluid-like properties under rest and low shear, but solid-like behavior at higher frequencies. Exploiting the unique genetic encodability of these materials, we demonstrate the assembly of protein networks within living mammalian cells and show via fluorescence recovery after photobleaching (FRAP) that mechanical properties can be tuned intracellularly in a manner similar to formulations formed extracellularly. We anticipate that the ability to modularly construct and systematically program the viscoelastic properties of designer protein-based materials could have broad utility in biomedicine, with applications in tissue engineering, therapeutic delivery, and synthetic biology.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Viscoelastic Particle Focusing and Separation in a Spiral Channel

As one type of non-Newtonian fluid, viscoelastic fluids exhibit unique properties that contribute to particle lateral migration in confined microfluidic channels, leading to opportunities for particle manipulation and separation. In this paper, particle focusing in viscoelastic flow is studied in a wide range of polyethylene glycol (PEO) concentrations in aqueous solutions. Polystyrene beads with diameters from 3 to 20 μm are tested, and the variation of particle focusing position is explained by the coeffects of inertial flow, viscoelastic flow, and Dean flow. We showed that particle focusing position can be predicted by analyzing the force balance in the microchannel, and that particle separation resolution can be improved in viscoelastic flows.

42 ENGINEERING↗

DOE OSTI2023

Thixotropy, antithixotropy, and viscoelasticity in hysteresis

Thixotropy, antithixotropy, and viscoelasticity are three types of time-dependent dynamics that involve fundamentally different underlying physical processes. Here, we show that the three dynamics exhibit different signatures in hysteresis by examining the fingerprints of the simplest thixotropic kinetic model, a new antithixotropic model that we introduce here, and the Giesekus model. We start by showing that a consistent protocol to generate hysteresis loops is a discrete shear-rate controlled ramp that begins and ends at high shear rates, rather than at low shear rates. Using this protocol, we identify two distinguishing features in the resulting stress versus shear rate loops. The first is the direction of the hysteresis loops: clockwise for thixotropy, but counterclockwise for viscoelasticity and antithixotropy. A second feature is achieved at high ramping rates where all responses lose hysteresis: the viscoelastic response shows a stress plateau at low shear rates due to lack of stress relaxation, whereas the thixotropic and antithixotropic responses are purely viscous with minimal shear thinning or thickening. We establish further evidence for these signatures by experimentally measuring the hysteresis of Laponite suspensions, carbon black suspensions, and poly(ethylene oxide) solutions, each representing a historically accepted example of each class of material behavior. The signatures measured in experiments are consistent with those predicted by the three models. This study reveals different fingerprints in hysteresis loops associated with thixotropy, antithixotropy, and viscoelasticity, which may be helpful in distinguishing the three time-dependent responses.

Mechanics↗

NASA NTRS1978

Postseismic surface deformations due to lithospheric and asthenospheric viscoelasticity

A model is proposed for post seismic surface deformations attributing them to lithospheric and asthenospheric viscoelasticity. The model predicts that the deformations due to lithospheric viscoelasticity depend on the ratio of the effective shear modulus acting long after the lithospheric viscoelastic relaxation to that acting immediately following the earthquake. While such deformations are generally smaller than those associated with asthenospheric viscoelasticity, they occur on a shorter time scale and may be in opposite direction to both the motion occurring at the time of the earthquake and that occurring as the asthenospheric relaxation occurs.

Cohen, S. C.↗

NASA NTRS1979

Postseismic viscoelastic deformation and stress. Part 2: Stress theory and computation; dependence of displacement, strain, and stress on fault parameters

A viscoelastic model for deformation and stress associated with earthquakes is reported. The model consists of a rectangular dislocation (strike slip fault) in a viscoelastic layer (lithosphere) lying over a viscoelastic half space (asthenosphere). The time dependent surface stresses are analyzed. The model predicts that near the fault a significant fraction of the stress that was reduced during the earthquake is recovered by viscoelastic softening of the lithosphere. By contrast, the strain shows very little change near the fault. The model also predicts that the stress changes associated with asthenospheric flow extend over a broader region than those associated with lithospheric relaxation even though the peak value is less. The dependence of the displacements, stresses on fault parameters studied. Peak values of strain and stress drop increase with increasing fault height and decrease with fault depth. Under many circumstances postseismic strains and stresses show an increase with decreasing depth to the lithosphere-asthenosphere boundary. Values of the strain and stress at distant points from the fault increase with fault area but are relatively insensitive to fault depth.

Cohen, S. C.↗

NASA NTRS1988

Numerical solution methods for viscoelastic orthotropic materials

Numerical solution methods for viscoelastic orthotropic materials, specifically fiber reinforced composite materials, are examined. The methods include classical lamination theory using time increments, direction solution of the Volterra Integral, Zienkiewicz's linear Prony series method, and a new method called Nonlinear Differential Equation Method (NDEM) which uses a nonlinear Prony series. The criteria used for comparison of the various methods include the stability of the solution technique, time step size stability, computer solution time length, and computer memory storage. The Volterra Integral allowed the implementation of higher order solution techniques but had difficulties solving singular and weakly singular compliance function. The Zienkiewicz solution technique, which requires the viscoelastic response to be modeled by a Prony series, works well for linear viscoelastic isotropic materials and small time steps. The new method, NDEM, uses a modified Prony series which allows nonlinear stress effects to be included and can be used with orthotropic nonlinear viscoelastic materials. The NDEM technique is shown to be accurate and stable for both linear and nonlinear conditions with minimal computer time.

Gramoll, K. C.↗

NASA NTRS1988

Thermo-viscoelastic analysis of composite materials, volume 1

Advanced composite materials, especially graphite/epoxy, are being applied to aircraft structures in order to improve performance and save weight. An important consideration in composite design is the residual strength of a structure containing holes, delaminations, or interlaminar damage when subjected to compressive loads. Recent studies have revealed the importance of viscoelastic effects in polymer-based composites. The viscoelastic effect is particularly significant at elevated temperature/moisture conditions since the matrix material is strongly affected by the environment. The solution of viscoelastic problems in composites was limited to special cases which can be solved by classical lamination theory. A finite element procedure is presented for calculating time-dependent stresses and strains in composite structures with general configurations and complicated boundary conditions. Using this procedure the in-plane and interlaminar stress distributions and histories in notched and unnotched composites were obtained for mechanical and thermal loads. Both two-dimensional and three-dimensional viscoelastic problems are analyzed. The effects of layup orientation and load spectrum on creep response and stress relaxation were also studied.

Lin, K. Y.↗

NASA NTRS1990

Analysis of elastically tailored viscoelastic damping member

For more than two decades, viscoelastic materials have been commonly used as a passive damping source in a variety of structures because of their high material loss factors. In most of the applications, viscoelastic materials are used either in series with or parallel to the structural load path. The latter is also known as the constrained-layer damping treatment. The advantage of the constrained-layer damping treatment is that it can be incorporated without loss in structural integrity, namely, stiffness and strength. However, the disadvantages are that: (1) it is not the most effective use of the viscoelastic material when compared with the series-type application, and (2) weight penalty from the stiff constraining layer requirement can be excessive. To overcome the disadvantages of the constrained-layer damping treatment, a new approach for using viscoelastic material in axial-type structural components, e.g., truss members, was studied in this investigation.

Chen, G.-S.↗

NASA NTRS1989

Recent results concerning the stability of viscoelastic shear deformable plates under compressive edge loading

Some recent results obtained by the authors are summarized concerning the stability of transversely isotropic flat panels whose materials exhibit a viscoelastic behavior and whose edges are subjected to in-plane biaxial compressive loads. Two transversely isotropic type materials, largely used in advanced technology, are considered: (1) the pyrolytic-graphite type, used in the thermal protection of aerospace vehicles, and (2) the type corresponding to unidirectional fiber-reinforced composites. In the former case, the planes of isotropy are parallel at each point to the midplane of the plate. In the latter case, they are normal to the fiber directions. The micromechanical relations developed by Aboudi (1984, 1986, 1987) are considered in conjunction with the correspondence principle of linear viscoelastic theory in order to predict the macroscopic viscoelastic properties of a material composed of uniaxial elastic fibers embedded in a linear viscoelastic matrix.

Librescu, L.↗

NASA NTRS1992

The viscoelastic characterization of polymer materials exposed to the low-Earth orbit environment

Recent accomplishments in our research efforts have included the successful measurement of the thermal mechanical properties of polymer materials exposed to the low-earth orbit environment. In particular, viscoelastic properties were recorded using the Rheometrics Solids Analyzer (RSA 2). Dynamic moduli (E', the storage component of the elastic modulus, and E'', the loss component of the elastic modulus) were recorded over three decades of frequency (0.1 to 100 rad/sec) for temperatures ranging from -150 to 150 C. Although this temperature range extends beyond the typical use range of the materials, measurements in this region are necessary in the development of complete viscoelastic constitutive models. The experimental results were used to provide the stress relaxation and creep compliance performance characteristics through viscoelastic correspondence principles. Our results quantify the differences between exposed and control polymer specimens. The characterization is specifically designed to elucidate a constitutive model that accurately predicts the change in behavior of these materials due to exposure. The constitutive model for viscoelastic behavior reflects the level of strain, the rate of strain, and the history of strain as well as the thermal history of the material.

Strganac, Thomas↗

NASA NTRS1995

The Singularity Mystery Associated with a Radially Continuous Maxwell Viscoelastic Structure

The singularity problem associated with a radially continuous Maxwell viscoclastic structure is investigated. A special tool called the isolation function is developed. Results calculated using the isolation function show that the discrete model assumption is no longer valid when the viscoelastic parameter becomes a continuous function of radius. Continuous variations in the upper mantle viscoelastic parameter are especially powerful in destroying the mode-like structures. The contribution to the load Love numbers of the singularities is sensitive to the convexity of the viscoelastic parameter models. The difference between the vertical response and the horizontal response found in layered viscoelastic parameter models remains with continuous models.

Fang, Ming↗

NASA NTRS2002

Nonlinear Viscoelastic Mechanics of Cross-linked Rubbers

The paper develops a general theory for finite rubber viscoelasticity, and specifies it in the form, convenient for solving problems important for rubber, tire and space industries. Based on the quasi-linear approach of non-equilibrium thermodynamics, a general nonlinear theory has been developed for arbitrary nonisothermal deformations of viscoelastic solids. In this theory, the constitutive equations are presented as the sum of known equilibrium (rubber elastic) and non-equilibrium (liquid polymer viscoelastic) terms. These equations are then simplified using several modeling arguments. Stability constraints for the proposed constitutive equations are also discussed. It is shown that only strong ellipticity criteria are applicable for assessing stability of the equations governing viscoelastic solids.

Freed, Alan D.↗

NASA NTRSDate not supplied

Variational Asymptotic Homogenization of Finitely Deformed Viscoelastic-Viscoplastic Composites

The objective of this paper is to develop a constitutive model for finitely deformed viscoelastic-viscoplastic materials and a micromechanics approach to homogenizing composites consisting of such materials. The development of the constitutive model involves establishing a thermodynamic framework based on finite strain theory, developing a viscoelasticity and a viscoplasticity model based on the thermodynamic framework, developing a radial return algorithm based on a classic framework, and deriving a closed-from incremental constitutive relation in the spatial configuration. The development of the micromechanics approach involves pulling-back the above constitutive relation to the material configuration, formulating a variational statement with the resulting constitutive relation, discretizing variational statement in a finite-dimensional space, and solving the discretized variational statement using an Euler–Newton predictor–corrector method. The constitutive model is calibrated via monotonic uniaxial compression tests on a polymer, and the calibrated model is validated by comparing its predictions with the cyclic test data. It is shown capable of characterizing viscoelasticity, viscoplasticity, and complex loading paths. The micromechanics approach’s capabilities are demonstrated through homogenizing a unidirectional fiber-reinforced composite, subjected to uniaxial, biaxial, and shear loading, at different strain rates. It is demonstrated to be capable of handling rate dependence and complex loading paths. The present framework can be further improved by implementing more sophisticated viscoelasticity and viscoplasticity models in future work.

Finite element analysis↗

DOE OSTI2021

Experimental workflow to estimate model parameters for evaluating long term viscoelastic response of CO2 storage caprocks

Understanding the time-dependent behavior of reservoir and sealing formations is critical to assessing risks associated with geological carbon storage since time-dependent deformation strongly influences mechanical responses of some rock types. Many studies have evaluated the risk of CO2 leakage and induced seismicity by assuming poroelastic rheology in sealing formations. Few have considered viscoelastic or other time-dependent responses, where the existing literature adopts 1D models to represent long-term time-dependent responses. This is primarily because to date, the general form of a reasonable 3D time-dependent model for rocks remains unclear. In this paper, we address this unclear issue by proposing a new workflow to select constitutive modeling parameters to evaluate if a 3D viscoelastic model is reasonable using several-hour-long experimental data and a power-law response to extrapolate to the decades-long time frames of interest in geologic carbon storage. To provide experimental data, we conducted multi-level loading/unloading triaxial relaxation tests with four rock types. The experimental results showed that the maximum load relaxation observed is approximately 49%, with some rock types showing as little as 1.4%. Using a simple linear viscoelastic model, parameters were chosen such that a maximum deviation of 1.5 MPa in axial stress and 7 MPa in radial stress was attained with the extrapolated 30-year data. We found that a reasonable parameter range for the normalized elastic modulus is 0.1~2 for rocks with significant time-dependent responses and 0.01~0.06 for those with small time-dependent responses. No matter how significant time-dependent responses are for rocks considered, our results showed that the relaxation time has a general range of 1~10^10 s, whose time scale can be one or two orders higher than a time frame typically envisioned for CO2 injection projects.

Stress relaxation, 3D time-dependent model, viscoe↗

DOE OSTI2023

Quasi‐dynamic breathing model of the lung incorporating viscoelasticity of the lung tissue

Abstract We advanced a novel model to calculate viscoelastic lung compliance and airflow resistance in presence of mucus, accounting for the quasi‐linear viscoelastic stress–strain response of the parenchyma (alveoli) tissue. We adapted a continuum‐based numerical modeling approach for the lung, integrating the fluid mechanics of the airflow within individual generations of the bronchi and alveoli. The model accounts for elasticity of the deformable bronchioles, resistance to airflow due to the presence of mucus within the bronchioles, and subsequent mucus flow. Simulated quasi‐dynamic inhalation and expiration cycles were used to characterize the net compliance and resistance of the lung, considering the rheology of the mucus and viscoelastic properties of the parenchyma tissue. The structure and material properties of the lung were identified to have an important contribution to the lung compliance and airflow resistance. The secondary objective of this work was to assess whether a higher frequency and smaller volume of harmonic air flow rate compared to a normal ventilator breathing cycle enhanced mucus outflow. Results predict, lower mucus viscosity and higher excitation frequency of breathing are favorable for the flow of mucus up the bronchi tree, towards the trachea.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2021

On the additive manufacturing (3D printing) of viscoelastic materials and flow behavior: From composites to food manufacturing

Additive manufacturing (AM) or more commonly known as 3D-printing has gained much ground in industrial manufacturing because of its breakthrough in rapid prototyping and processes. To date, the 3D-printing market has grown significantly and is poised for growth in line with digitization of manufacturing. Furthermore, the main objective of this review article focuses on the viscoelastic behavior (viscous solution) of 3D printing materials at ambient conditions, which are not essentially under melt-flow or higher temperatures. The initial section reviews the basic concepts on viscosity and viscoelastic phenomenon, with emphasis on the preferred conditions a viscous material should have prior to 3D-printing. Several examples of structures formed from viscoelastic materials through 3D-printing are also detailed, as well as the various curing techniques for different printed objects or models. While there is much interest on industrial applications, the last part surveys various food formulations used for 3D-printing.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Molecular origin of viscoelasticity and influence of methylation in mesophase pitch

The viscoelastic and thermomechanical properties of pitches are responsible for their melt-spinning behavior, which is a critical step for manufacturing high-performance pitch-based carbon fibers. Here, we systematically explore the impact of methyl group modifications on the viscoelastic and thermal properties of mesophase pitches. We employ a range of atomistic modeling approaches, including Density Functional Theory (DFT), Density Functional Tight Binding (DFTB), and Classical Molecular Mechanics (MM), to provide detailed insights into the molecular interactions and structural changes. Further, our results revealed the molecular mechanisms that promote layered structures leading to the anisotropic nature of the viscoelastic behavior of mesophase pitch. Furthermore, we propose a modified molecular representation of naphthalene-based mesophase pitch based on the analysis of x-ray diffraction measurements. This study provides fundamental insights into the molecular structures of mesophase pitch and the role of methyl groups controlling its viscosity, which offer valuable insights into mesophase-based carbon fiber production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Effect of Diphenyl Content on Viscoelasticity of Poly(dimethyl- co -diphenyl)siloxane Melt and Network

Polydimethylsiloxane (PDMS) is one of the most widely used polymeric materials for sealants, adhesives, lubricants, and thermal as well as electrical insulation. At low temperatures, however, PDMS is subject to crystallization that can cause deterioration in mechanical function. A common way to suppress such crystallization is through the incorporation of phenylsiloxane into the backbone of polysiloxane. Nevertheless, the introduction of phenyl components, even in small quantities, could potentially change the properties of the siloxane in a significant way. In this work, a series of mechanical tests and finite element simulations were performed to study the macroscale viscoelasticity of two poly(dimethyl-co-diphenyl)siloxane formulations in order to understand the effects of a few percent diphenyl contents on the viscoelasticity of the polysiloxane material. Here, we utilized the small-angle X-ray scattering to investigate the microscopic structures of the copolymers and broadband dielectric spectroscopy and rheology to probe the chain dynamics at the microscale. The results of these characterizations were used to inform the finite element simulations. We found that the degree of cross-linking does not significantly alter the microstructure but can profoundly affect the viscoelastic response of the copolymer networks. The corresponding hysteretic behavior is interpreted in terms of reptation-like motion and relaxation of the effective free chains in the cured polymer network. The relaxation of the copolymer chains is slowed significantly by even a small increase in the molar ratio of the diphenyl component.

36 MATERIALS SCIENCE↗