Controlling Magnetization Reversal and Hyperthermia Efficiency in Core–Shell Iron–Iron Oxide Magnetic Nanoparticles by Tuning the Interphase Coupling

[Image: see text] Magnetic particle hyperthermia, in which colloidal nanostructures are exposed to an alternating magnetic field, is a promising approach to cancer therapy. Unfortunately, the clinical efficacy of hyperthermia has not yet been optimized. Consequently, routes to improve magnetic particle hyperthermia, such as designing hybrid structures comprised of different phase materials, are actively pursued. Here, we demonstrate enhanced hyperthermia efficiency in relatively large spherical Fe/Fe-oxide core–shell nanoparticles through the manipulation of interactions between the core and shell phases. Experimental results on representative samples with diameters in the range 30–80 nm indicate a direct correlation of hysteresis losses to the observed heating with a maximum efficiency of around 0.9 kW/g. The absolute particle size, the core–shell ratio, and the interposition of a thin wüstite interlayer are shown to have powerful effects on the specific absorption rate. By comparing our measurements to micromagnetic calculations, we have unveiled the occurrence of topologically nontrivial magnetization reversal modes under which interparticle interactions become negligible, aggregates formation is minimized and the energy that is converted into heat is increased. This information has been overlooked until date and is in stark contrast to the existing knowledge on homogeneous particles.