Non-Altermagnetic Origin of Exchange Bias Behaviors in Incoherent RuO₂/Fe Bilayer Heterostructures

Initially identified as a promising altermagnetic (AM) candidate, rutile RuO₂ has since become embroiled in controversy due to contradictory findings of modeling and measurements of the magnetic properties of bulk crystals and thin films. For example, despite observations of a bulk non-magnetic state using density functional theory, neutron scattering, and muon spin resonance measurements, patterned RuO₂ Hall bars and film heterostructures display magnetotransport signatures of magnetic ordering. Among the characteristics routinely cited as evidence for AM is the observation of exchange bias (EB) in an intimately contacted Fe-based ferromagnetic (FM) layer, which can arise due to interfacial coupling with a compensated antiferromagnet. Within this work, the origins of this EB coupling in Ru-capped RuO₂/Fe bilayers are investigated using polarized neutron diffraction, polarized neutron reflectometry, cross-sectional transmission electron microscopy, and super conducting quantum interference device measurements. These experiments reveal that the EB behavior is driven by the formation of an iron oxide interlayer containing Fe₃O₄ that undergoes a magnetic transition and pins interfacial moments within Fe at low temperature. These findings are confirmed by comparable measurements of Ni-based heterostructures, which do not display EB coupling, as well as magnetometry of additional Fe/Ru bilayers that display oxide-driven EB coupling despite the absence of the epitaxial RuO₂ layer. While these results do not directly refute the possibility of AM ordering in RuO₂ thin films, they reveal that EB, and related magnetotransport phenomena, cannot alone be considered evidence of this characteristic in the rutile structure due to interfacial chemical disorder.