Structure-Property Relationships via Recovery Rheology in Viscoelastic Materials

The recoverable strain is shown to correlate to the temporal evolution of microstructure via time-resolved small-angle neutron scattering and dynamic shear rheology. Investigating two distinct polymeric materials of wormlike micelles and fibrin network, we demonstrate that, in addition to the nonlinear structure-property relationships, the shear and normal stress evolution is dictated by the recoverable strain. A distinct sequence of physical processes under large amplitude oscillatory shear (LAOS) is identified that clearly contains information regarding both the steady-state flow curve and the linear-regime frequency sweep, contrary to most interpretations that LAOS responses are either distinct from or somehow intermediate between the two cases. This work provides a physically motivated and straightforward path to further explore the structure-property relationships of viscoelastic materials under dynamic flow conditions.