Abstract
Large amplitude oscillatory shear strain was applied to anionically synthesized linear polystyrene solutions in dioctylphthalate. The resulting torque was analyzed in Fourier space with respect to frequency, magnitude, and phase (Fourier-transform rheology). The concentration of the solutions was varied to achieve different degrees of entanglement. In addition, numerical simulations were performed using the Giesekus constitutive equation fitted on the basis of linear viscoelastic data. We found a good qualitative agreement between experiments and predictions; a quantitative agreement was reached for intermediate strain amplitudes. Some deviations were observed at very low strain amplitudes. We present a descriptive relation for the relative magnitude of the third harmonic as a function of strain amplitude using a modified damping function. From this relation we obtained a universal parameter that describes the scaling behavior law for the increasing non-linearity (e.g., measured by the relative intensity ...
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