Enhanced hardening of soft self-assembled copolymer gels under homogeneous magnetic fields

The rheological response of highly swollen physical gels obtained by self-assembling of triblock copolymers containing low remanence ferromagnetic particles was investigated in the presence of external homogeneous magnetic fields. Three different types of sample geometries with distinctive magnetic particle orderings were investigated: isotropic (no magnetic field present during synthesis), parallel to the plane of the gel film and perpendicular to the plane of the gel film. Both the storage and loss moduli exhibit a strong increase with magnetic field strength for all geometries. Dependence of the rheological response on particle volume fraction was also investigated. The strength of such rheological hardening, as well as its saturation behaviour, depend strongly on the relative orientation between particle strings, shear and external field. In some cases a very strong relative increase of storage modulus, up to 6000% was obtained. Further transient rheological studies suggest that strong rearrangement of the particle network is largely responsible for the enormous increase in elastic modulus. Parallel to that, a maximum in the loss factor was observed as a function of particle volume fraction and field strength and it was interpreted in terms of a competition between an increase in string (clusters) hardening and a decrease in their ability to deform and flow. These results suggest that magnetorheological gels are an intermediate system between magnetorheological elastomers (MREs) and magnetorheological fluids (MRFs) with directional dependent rheological response and partial rearrangement of the particle network.