Magnetic-Field-Assisted Assembly of Anisotropic Superstructures by Iron Oxide Nanoparticles and Their Enhanced Magnetism

Magnetic nanoparticle superstructures with controlled magnetic alignment and desired structural anisotropy hold promise for applications in data storage and energy storage. Assembly of monodisperse magnetic nanoparticles under a magnetic field could lead to highly ordered superstructures, providing distinctive magnetic properties. In this work, a low-cost fabrication technique was demonstrated to assemble sub-20-nm iron oxide nanoparticles into crystalline superstructures under an in-plane magnetic field. The gradient of the applied magnetic field contributes to the anisotropic formation of micron-sized superstructures. The magnitude of the applied magnetic field promotes the alignment of magnetic moments of the nanoparticles. The strong dipole-dipole interactions between the neighboring nanoparticles lead to a close-packed pattern as an energetically favorable configuration. Rod-shaped and spindle-shaped superstructures with uniform size and controlled spacing were obtained using spherical and polyhedral nanoparticles, respectively. The arrangement and alignment of the superstructures can be tuned by changing the experimental conditions. The two types of superstructures both show enhancement of coercivity and saturation magnetization along the applied field direction, which is presumably associated with the magnetic anisotropy and magnetic dipole interactions of the constituent nanoparticles and the increased shape anisotropy of the superstructures. Our results show that the magnetic-field-assisted assembly technique could be used for fabricating nanomaterial-based structures with controlled geometric dimensions and enhanced magnetic properties for magnetic and energy storage applications.