Characterization of the material behavior and identification of effective elastic moduli based on molecular dynamics simulations of coarse-grained silica

“The addition of fillers can significantly improve the mechanical behavior of polymers. The responsible mechanisms at the molecular level can be well assessed by particle-based simulation techniques, such as molecular dynamics. However, the high computational cost of these simulations prevents the study of macroscopic samples. Continuum-based approaches, particularly micromechanics, offer a more efficient alternative but require precise constitutive models for all constituents, which are usually unavailable at these small length scales. In this contribution, we derive a molecular-dynamics-informed constitutive law by employing a characterization strategy introduced in a previous publication. We choose silicon dioxide (silica) as an exemplary filler material used in polymer composites and perform uniaxial and shear deformation tests with molecular dynamics. The material exhibits elastoplastic behavior with a pronounced anisotropy. Based on the pseudo-experimental data, we calibrate an anisotropic elastic constitutive law and reproduce the material response for small strains accurately. The study validates the characterization strategy that facilitates the calibration of constitutive laws from molecular dynamics simulations. Furthermore, the obtained material model for coarse-grained silica forms the basis for future continuum-based investigations of polymer nanocomposites. In general, the presented transition from a fine-scale particle model to a coarse and computationally efficient continuum description adds to the body of knowledge of molecular science as well as the engineering community.”