Effect of Particle Mobility and Preformed Microstructure on Magnetoelectric Coupling of Two‐Layer PEP ‐ MAE Composites

ABSTRACT In this work, we investigate how the preformed microstructure and field‐induced particles' mobility in magnetoactive elastomers (MAE) influence magnetoelectric coupling in two‐layer structures composed of a piezoelectric polymer (PEP) film and a MAE layer. In anisotropic MAE, iron microparticles are pre‐aligned into chains oriented perpendicular to the sample plane, defining the magnetic “easy axis.” The structural anisotropy enhances the resonance mechanical deformation of the MAE layer under a gradient AC magnetic field, thereby amplifying the electric response induced in the PEP layer. Both the magnetoelectric effect (MEE) coefficient and resonance frequency are found to depend strongly on matrix elasticity and the resulting particle mobility even at a fixed filler concentration. In contrast, the MEE remains insensitive to changes in the polymer's elastic properties in PEP‐MAE with anisotropic structure, confirming the stability of preformed chains under field exposure. These findings demonstrate that tailoring the internal architecture of the MAE layer enables precise control over the MEE characteristics, offering a robust route to optimize flexible magnetoelectric devices for applications in sensing, energy harvesting, and biomedicine.