Magneto-elastic coupling as a key to microstructural response of magnetic elastomers with flake-like particles.

Using the combination of experiment and molecular dynamics simulations, we investigate structural transformations in magnetic elastomers with NdFeB flake-like particles, caused by applied moderate magnetic fields. We explain why and how those transformations depend on whether or not the samples are initially cured by a short-time exposure to a strong field. We find that in a cured sample, a moderate magnetic field leads mainly to in-place flake rotations that are fully reversed once the applied field is switched off. In contrast, in an initially non-cured sample the flakes perform both translation and rotations under the influence of a moderate applied field that lead to the formation of chain-like structures that remain such even if the field is switched off.

Tunable dynamic moduli of magnetic elastomers: from characterization by x-ray micro-computed tomography to mesoscopic modeling.

Ferrogels and magnetorheological elastomers are composite materials obtained by embedding magnetic particles of mesoscopic size in a crosslinked polymeric matrix. They combine the reversible elastic deformability of polymeric materials with the high responsivity of ferrofluids to external magnetic fields. These materials stand out, for example, for significant magnetostriction as well as a pronounced increase of the elastic moduli in the presence of external magnetic fields. By means of x-ray micro-computed tomography, the position and size of each magnetic particle can be measured with a high degree of accuracy. We here use data extracted from real magnetoelastic samples as input for coarse-grained dipole-spring modeling and calculations to investigate internal restructuring, stiffening, and changes in the normal modes spectrum. More precisely, we assign to each particle a dipole moment proportional to its volume and set a randomized network of springs between them that mimics the behavior of the polymeric elastic matrix. Extending our previously developed methods, we compute the resulting structural changes in the systems as well as the frequency-dependent elastic moduli when magnetic interactions are turned on. Particularly, with increasing magnetization, we observe the formation of chain-like aggregates. Interestingly, the static elastic moduli can first show a slight decrease with growing amplitude of the magnetic interactions, before a pronounced increase appears upon the chain formation. The change of the dynamic moduli with increasing magnetization depends on the frequency and can even feature nonmonotonic behavior. Overall, we demonstrate how theory and experiments can complement each other to learn more about the dynamic behavior of this interesting class of materials.