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We report nanoscale inter-particle magnetic orderings in self-assemblies ofFe3O4 nanoparticles (NPs), and the emergence of inter-particleantiferromagnetic (AF) (super-antiferromagnetic) correlations near the coercivefield at low temperature. The magnetic ordering is probed via x-ray resonantmagnetic scattering (XRMS), with the x-ray energy tuned to the Fe-L3 edge andusing circular polarized light. By exploiting dichroic effects, a magneticscattering signal is isolated from the charge scattering signal. The magneticsignal informs about nanoscale spatial orderings at various stages throughoutthe magnetization process and at various temperatures throughout thesuperparamagnetic blocking transition, for two different sizes of NPs, 5 and 11nm, with blocking temperatures TB of 28 K and 170 K, respectively. At 300 K,while the magnetometry data essentially shows superparamagnetism and absence ofhysteresis for both particle sizes, the XRMS data reveals the presence ofnon-zero (up to 9/100) inter-particle AF couplings when the applied field isreleased to zero for the 11 nm NPs. These AF couplings are drasticallyamplified when the NPs are cooled down below TB and reach up to 12/100 for the5 nm NPs and 48/100 for the 11 nm NPs, near the coercive point. The datasuggests that the particle size affects the prevalence of the AF couplings:compared to ferromagnetic (F) couplings, the relative prevalence of AFcouplings at the coercive point increases from a factor ~ 1.6 to 3.8 when theNP size increases from 5 to 11 nm.

Emergent super-antiferromagnetic correlations in monolayers of Fe3O4 nanoparticles throughout the superparamagnetic blocking transition