Unraveling the Effect of Strain Rate and Temperature on the Heterogeneous Mechanical Behavior of Polymer Nanocomposites via Atomistic Simulations and Continuum Models

Polymer nanocomposites are characterized by heterogeneous mechanical behavior and performance, which is mainly controlled by the interaction between the nanofiller and the polymer matrix. Optimizing their material performance in engineering applications requires understanding how both the temperature and strain rate of the applied deformation affect mechanical properties. This work investigates the effect of strain rate and temperature on the mechanical properties of poly(ethylene oxide)/silica (PEO/SiO₂) nanocomposites, revealing their behavior in both the melt and glassy states, via atomistic molecular dynamics simulations and continuum models. In the glassy state, the results indicate that Young’s modulus increases by up to 99.7% as the strain rate rises from 1.0 × 10⁻⁷ fs⁻¹ to 1.0 × 10⁻⁴ fs⁻¹, while Poisson’s ratio decreases by up to 39.8% over the same range. These effects become even more pronounced in the melt state. Conversely, higher temperatures lead to an opposing trend. A local, per-atom analysis of stress and strain fields reveals broader variability in the local strain of the PEO/SiO₂ nanocomposites as temperature increases and/or the deformation rate decreases. Both interphase and matrix regions lose rigidity at higher temperatures and lower strain rates, blurring their distinctiveness. The results of the atomistic simulations concerning the elastic modulus and Poisson’s ratio are in good agreement with the predictions of the Richeton–Ji model. Additionally, these findings can be leveraged to design advanced polymer composites with tailored mechanical properties and could optimize structural components by enhancing their performance under diverse engineering conditions.