A finite viscoelastic constitutive model for low to high strain rate response of elastomers with application of strain rate-induced glass transition

TL;DR

This paper introduces a thermodynamically consistent, micromechanically-inspired constitutive model for elastomers that captures rate-dependent behavior and glass transition phenomena across a wide range of strain rates, validated by experiments and simulations.

Contribution

The authors develop a novel constitutive model that integrates viscous flow and molecular rearrangement to predict elastomer behavior from low to high strain rates, including glass transition effects.

Findings

Model predicts increased energy dissipation with strain rate.

Molecular relaxation dissipation decreases beyond a crossover rate.

Accurately captures storage and loss modulus behavior across frequencies.

Abstract

Amorphous elastomers exhibit significant rate-stiffening and unique viscous flow characteristics across a wide range of strain rates, often undergoing glass transition above a strain rate threshold. We have developed a thermodynamically-consistent and micromechanically-inspired constitutive model for soft elastomeric materials to capture the rate-dependent stress-strain behavior and hysteresis when subjected to low to high strain rates. Our proposed constitutive model encapsulates the viscous flow of materials through molecular motion at low strain rates and local rearrangement and alignment at high strain rates, essentially covering the glass transition. We applied our constitutive model to uniaxial compression experiments performed at low and high strain rates for polyborosiloxane (PBS) to identify the material parameters, and subsequently, performed numerical simulations of single and multi-cycle compression, stress relaxation, and small amplitude oscillatory tension-compression. Our analyses indicate that the model predicts higher total energy dissipation with increasing strain rate; however, dissipation associated with molecular relaxation decreases (forming a cusp) because, beyond a crossover strain rate, molecular rearrangement and alignment become dominant, which is consistent with the onset of the glass transition. For cyclic loading-unloading, we observed that dissipation over a cycle remains constant at low strain rate but decreases non-monotonically at high strain rates before becoming constant with peak stress over the cycle becoming higher, which can be interpreted as more loading being carried elastically by the polymer network as the molecular rearrangement process occurs. Additionally, our model was able to predict the qualitative nature of the storage modulus and loss modulus in the limit of small strain over a wide range of frequency sweeps.