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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. 

The magnetic proximity effect (MPE) has recently been explored to manipulate interfacial properties of two-dimensional (2D) transition metal dichalcogenide (TMD)/ferromagnet heterostructures for use in spintronics and valleytronics. However, a full understanding of the MPE and its temperature and magnetic field evolution in these systems is lacking. In this study, the MPE has been probed in Pt/WS2/BPIO (biphase iron oxide, Fe3O4 and α-Fe2O3) heterostructures through a comprehensive investigation of their magnetic and transport properties using magnetometry, four-probe resistivity, and anomalous Hall effect (AHE) measurements. Density functional theory (DFT) calculations are performed to complement the experimental findings. We found that the presence of monolayer WS2 flakes reduces the magnetization of BPIO and hence the total magnetization of Pt/WS2/BPIO at T > ~120 K—the Verwey transition temperature of Fe3O4 (TV). However, an enhanced magnetization is achieved at T < TV. In the latter case, a comparative analysis of the transport properties of Pt/WS2/BPIO and Pt/BPIO from AHE measurements reveals ferromagnetic coupling at the WS2/BPIO interface. Our study forms the foundation for understanding MPE-mediated interfacial properties and paves a new pathway for designing 2D TMD/magnet heterostructures for applications in spintronics, opto-spincaloritronics, and valleytronics.