Manipulating magnetic anisotropy
(MA) purposefully in transition
metal oxides (TMOs) enables the development of oxide-based spintronic
devices with practical applications. Here, we report a pathway to
reversibly switch the lateral magnetic easy-axis via interfacial oxygen
octahedral coupling (OOC) effects in 3d–5d tricolor superlattices,
i.e., [SrIrO3,mRTiO3,SrIrO3,2La0.67Sr0.33MnO3]10 (RTiO3: SrTiO3 and CaTiO3). In the heterostructures,
the anisotropy energy (MAE) is enhanced over one magnitude to ∼106 erg/cm3 compared to La0.67Sr0.33MnO3 films. Moreover, the magnetic easy-axis is reversibly
reoriented between (100) and (110) directions by changing the RTiO3. Using first-principles density functional theory calculations,
we find that the SrIrO3 owns a large single-ion anisotropy
due to its strong spin–orbit interaction. This anisotropy can
be reversibly controlled by the OOC and then reorient the easy-axis
of the superlattices. Additionally, it enlarges the MAE of the films
via the cooperation with a robust orbital hybridization between the
Ir and Mn atoms. Our results indicate that the tricolor superlattices
consisting of 3d and 5d oxides provide a powerful platform to study
the MA and develop oxide-based spintronic devices.