Controlled Close-Packing of Ferrimagnetic Nanoparticles: An Assessment of the Role of Interparticle Superexchange Versus Dipolar Interactions

The fundamental question as to the relative importance of interparticle superexchange versus dipolar interaction between oxide magnetic particles in direct physical contact is addressed by examining the magnetic. properties of a series of compacted samples comprising identical maghemite particles (8 nm in diameter) coated by nonmagnetic shells (oleic acid or silica) of varying thickness that control the distance between the magnetic cores and hence the packing density (particle volume fraction). A remarkably narrow maghemite particle size distribution is established by electron microscopy and small-angle X-ray scattering. The series includes a sample made up of bare particles in a random-close-packed configuration (therefore in direct contact) that exhibits ideal superspin-glass behavior with a relatively high freezing transition temperature. It is shown that interparticle superexchange interactions between the nanoparticles in this sample play a minor role compared to classical dipolar interactions in establishing the collective, superspin-glass state. This follows from the freezing temperature of the most concentrated samples in the series (those with 0 <= shell thickness < 3 nm), which are found to vary in direct proportionality with the volume fraction of the maghemite cores and therefore with the strength of dipolar interactions.