On the magnetoelectric performance of multiferroic particulate composite materials

In the current work, quantitative analysis of magnetoelectric particulate composite material system explicated the main mechanisms responsible for the below-optimal performance of this class of materials. We considered compliant particulate composite materials, with constituents relevant to technological and scientific interest, leading to 0–3 Terfenol-D/PVDF–TrFE composite samples. To this objective, thick Terfenol-D/PVDF–TrFE films (10–15 µm) were fabricated and analyzed for chemical, mechanical, and magnetic properties to demonstrate their suitability for energy applications in harsh environmental conditions. The vigorous experimental characterization of the composite exemplified the multifunctional properties, quantifying the interrelationship between the composition and performance. We observed that the addition of magnetic particles to the electroactive copolymer matrix resulted in improvement in the mechanical and electrical properties since the particles acted as pinning sites, hindering the deformation of the chains and enhancing polarization. The effective modulus model was amended to account for the crystallization-induced change in material stiffness. We also measured and computed the magnetic particles motion to explicate the detrimental effect of mobility and migration on the overall magnetoelectric coupling performance of the composite. Thereby, we derived an analytical model based on the magnetic force due to the co-presence of alternating and constant magnetic fields, and the viscous drag force due to the viscoelastic properties of the electroactive copolymer matrix. We demonstrated that the mobility of the particles plays a crucial role in the short and long term performance of magnetoelectric coupling in multiferroic particulate composites, uncovering the underpinnings of the dichotomy in performance between experimentally measured and analytically predicted coupling coefficients, thus allowing for the proposal of new approaches to realize the scientific potential of magnetoelectric particulate composites in energy applications.