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.