Search for: All records

We investigate the spatial distribution of spin orientation in magnetic nanoparticles consisting of hard and soft magnetic layers. The nanoparticles are synthesized in a core–shell spherical morphology where the target stoichiometry of the magnetically hard, high anisotropy layer is CoFe2O4 (CFO), while the synthesis protocol of the lower anisotropy material is known to produce Fe3O4. The nanoparticles have a mean diameter of ∼9.2–9.6 nm and are synthesized as two variants: a conventional hard/soft core–shell structure with a CFO core/FO shell (CFO@FO) and the inverted structure FO core/CFO shell (FO@CFO). High-resolution electron microscopy confirms the coherent spinel structure across the core–shell boundary in both variants, while magnetometry indicates the nanoparticles are superparamagnetic at 300 K and develop a considerable anisotropy at reduced temperatures. Low-temperature M vs H loops suggest a multistep reversal process. Small angle neutron scattering (SANS) with full polarization analysis reveals a considerable alignment of the spins perpendicular to the field even at fields approaching saturation. The perpendicular magnetization is surprisingly correlated from one nanoparticle to the next, though the interaction is of limited range. More significantly, the SANS data reveal a pronounced difference in the reversal process of the magnetization parallel to the field for the two nanoparticle variants. For the CFO@FO nanoparticles, the core and shell magnetizations appear to track each other through the coercive region, while in the FO@CFO variant, the softer Fe3O4 core reverses before the higher anisotropy CoFe2O4 shell, consistent with expectations from mesoscale magnetic modeling. These results highlight the interplay between interfacial exchange coupling and anisotropy as a means to tune the composite properties of the nanoparticles for tailored applications including biomedical/theranostic uses. 

We present an exploration of a family of compositionally complex cubic spinel ferrites featuring combinations of Mg, Fe, Co, Ni, Cu, Mn, and Zn cations, systematically investigating the average and local atomic structures, chemical short-range order, magnetic spin configurations, and magnetic properties. All compositions result in ferrimagnetic average structures with extremely similar local bonding environments; however, the samples display varying degrees of cation inversion and, therefore, differing apparent bulk magnetization. Additionally, first-order reversal curve analysis of the magnetic reversal behavior indicates varying degrees of magnetic ordering and interactions, including potentially local frustration. Finally, reverse Monte Carlo modeling of the spin orientation demonstrates a relationship between the degree of cation inversion and the spin collinearity. Collectively, these observations correlate with differences in synthesis procedures. This work provides a framework for understanding magnetic behavior reported for “high-entropy spinels,” revealing many are likely compositionally complex oxides with differing degrees of chemical short-range order—not meeting the community established criteria for high or medium entropy compounds. Moreover, this work highlights the importance of reporting complete sample processing histories and investigating local to long-range atomic arrangements when evaluating potential entropic mixing effects and assumed property correlations in high entropy materials.