Iron oxide nanoparticles have tremendous scientific and technological potential in a broad range of technologies, from energy applications to biomedicine. To improve their performance, single‐crystalline and defect‐free nanoparticles have thus far been aspired. However, in several recent studies, defect‐rich nanoparticles outperform their defect‐free counterparts in magnetic hyperthermia and magnetic particle imaging (MPI). Here, an overview on the state‐of‐the‐art of design and characterization of defects and resulting spin disorder in magnetic nanoparticles is presented with a focus on iron oxide nanoparticles. The beneficial impact of defects and disorder on intracellular magnetic hyperthermia performance of magnetic nanoparticles for drug delivery and cancer therapy is emphasized. Defect‐engineering in iron oxide nanoparticles emerges to become an alternative approach to tailor their magnetic properties for biomedicine, as it is already common practice in established systems such as semiconductors and emerging fields including perovskite solar cells. Finally, perspectives and thoughts are given on how to deliberately induce defects in iron oxide nanoparticles and their potential implications for magnetic tracers to monitor cell therapy and immunotherapy by MPI.

Magnetospirillum gryphiswaldense is a microorganism with the ability to biomineralize magnetite nanoparticles, called magnetosomes, and arrange them into a chain that behaves like a magnetic compass. Rather than straight lines, magnetosome chains are slightly bent, as evidenced by electron cryotomography. Our experimental and theoretical results suggest that due to the competition between the magnetocrystalline and shape anisotropies, the effective magnetic moment of individual magnetosomes is tilted out of the [111] crystallographic easy axis of magnetite. This tilt does not affect the direction of the chain net magnetic moment, which remains along the [111] axis, but explains the arrangement of magnetosomes in helical-like shaped chains. Indeed, we demonstrate that the chain shape can be reproduced by considering an interplay between the magnetic dipolar interactions between magnetosomes, ruled by the orientation of the magnetosome magnetic moment, and a lipid/protein-based mechanism, modeled as an elastic recovery force exerted on the magnetosomes.

The review presents the recent advances in small-angle scattering techniques for the characterization of magnetic nanoparticles and highlights the potential of these methods to facilitate the application-oriented nanoparticle design & synthesis.

The structural and magnetic properties of magnetic multi-core particles were determined by numerical inversion of small angle scattering and isothermal magnetisation data. The investigated particles consist of iron oxide nanoparticle cores (9 nm) embedded in poly(styrene) spheres (160 nm). A thorough physical characterisation of the particles included transmission electron microscopy, X-ray diffraction and asymmetrical flow field-flow fractionation. Their structure was ultimately disclosed by an indirect Fourier transform of static light scattering, small angle X-ray scattering and small angle neutron scattering data of the colloidal dispersion. The extracted pair distance distribution functions clearly indicated that the cores were mostly accumulated in the outer surface layers of the poly(styrene) spheres. To investigate the magnetic properties, the isothermal magnetisation curves of the multi-core particles (immobilised and dispersed in water) were analysed. The study stands out by applying the same numerical approach to extract the apparent moment distributions of the particles as for the indirect Fourier transform. It could be shown that the main peak of the apparent moment distributions correlated to the expected intrinsic moment distribution of the cores. Additional peaks were observed which signaled deviations of the isothermal magnetisation behavior from the non-interacting case, indicating weak dipolar interactions.