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In this work, we subject elastomers to a fixed pre-stretch in uniaxial extension, e p , upon which a large-amplitude, e 0, oscillatory uniaxial extensional (LAOE) deformation is superposed. We find that if both e p and e 0 are large enough, the stress responds with a rich set of higher harmonics, both even and odd. We further find the Lissajous-Bowditch plots of our measured stress responses versus uniaxial strain to be without twofold symmetry and, specifically, to be shaped like convex bananas. Our new continuum model for this behavior combines a new nonlinear spring, in parallel with a Newtonian dashpot, and we call this the Voigt model with strain-hardening. We consider this three-parameter (Young’s modulus, viscosity, and strain-hardening coefficient) model to be the simplest relevant one for the observed convex bananas. We fit the parameters to both our LAOE measurements and then to our uniaxial elongation measurements at constant extension rate. We develop analytical expressions for the Fourier components of the stress response, parts both in-phase and out-of-phase with the extensional strain, for the zeroth, first, second, and third harmonics. We find that the part of the second harmonic that is out-of-phase with the strain must be negative for proper banana convexity.

Analytical solutions for either the shear stress or the normal stress differences in large-amplitude oscillatory shear flow, both for continuum or molecular models, often take the form of the first few terms of a power series in the shear rate amplitude. Here, we explore improving the accuracy of these truncated series by replacing them with ratios of polynomials. Specifically, we examine replacing the truncated series solution for the corotational Maxwell model with its Pade approximants for the shear stress response and for the normal stress differences. We find these Pade approximants to agree closely with the corresponding exact solution, and we learn that with the right approximants, one can nearly eliminate the inaccuracies of the truncated expansions.

In small amplitude oscillatory shear flow, we now universally represent the response of a viscoelastic fluid as a complex quantity, which we call “complex viscosity.” This short piece deepens our understanding of the origins of the complex viscosity and of the man who coined this term, now widely used in rheology.

Using the integral form of a nonlinear corotational model, we derive explicit analytical expressions for the zeroth, second, and fourth harmonics of the second normal stress difference in large-amplitude oscillatory shear (LAOS). This model yields an arbitrary normal stress ratio (ANSR) in any simple shearing deformation, including LAOS. This corotational ANSR model adds one parameter to the corotational Maxwell model, a time constant λ 0 controlling the ratio Ψ2/Ψ1 for both the real and imaginary parts of each harmonic of the normal stress difference. The explicit analytical expressions for all harmonics of the alternating shear stress and first normal stress difference responses in LAOS match those obtained previously for the corotational Maxwell model. We evaluate the corotational ANSR model for the case of a single Maxwell relaxation time fluid.

Homogeneous shearing is required in sliding plate flow experiments with one plate fixed and the other oscillating. However, when fluid inertia becomes significant, the velocity gradient and the stress will not be uniform. MacDonald et al. (1969) and Schrag (1977) investigated this effect for a linear viscoelastic fluid. However, linear viscoelasticity does not describe the behavior of melts in large amplitude oscillatory shear (LAOS). Jeyaseelan et al. (1993) have shown that the Berkeley kinetic network model does accurately describe the LAOS behavior of polymer melts. In this work, the Berkeley model is solved for LAOS in sliding plate flow with fluid inertia, by numerical integration of spatially discretized forms of the governing equations. Nonlinear viscoelasticity is predicted to aggravate the effects of fluid inertia in LAOS and experiments confirm this. Specifically, fluid inertia amplifies the first harmonic and produces no even harmonics. Operating limits are presented graphically for minimizing inertial effects in LAOS experiments.

Large amplitude oscillatory shear (LAOS) flow has been used to characterize the nonlinear viscoelasticity of polymer melts and solutions. Results are frequently reported with shear stress versus strain loops, or with shear stress versus shear rate loops. A Fourier analysis of the stress response to LAOS is often desired for comparison with theory, or for quantitative comparison between resins. A method is presented which employs the discrete Fourier transform to obtain the Fourier series coefficients from LAOS loops.