Tuning Interfacial Ferromagnetism in LaNiO₃/CaMnO₃ Superlattices by Stabilizing Non-Equilibrium Crystal Symmetry

Perovskite oxide heterostructures offer an important path forward for stabilizing and controlling low-dimensional magnetism. One of the guiding design principles for these materials systems is octahedral connectivity. In superlattices composed of perovskites with different crystal symmetries, variation of the relative ratio of the constituent layers as well as the individual layer thicknesses gives rise to non-equilibrium crystal symmetries that, in turn, lead to unprecedented control of interfacial ferromagnetism. We have found that in superlattices of CaMnO$_3$ (CMO) and LaNiO$_3$ (LNO), interfacial ferromagnetism can be modulated by a factor of three depending on LNO and CMO layer thicknesses as well as their relative ratio. Such an effect is only possible due to the non-equilibrium crystal symmetries at the interfaces and can be understood in terms of the anisotropy of the exchange interactions and modifications in the interfacial Ni-O-Mn and Mn-O-Mn bond angles and lengths with increasing LNO layer thickness. These results demonstrate the potential of engineering non-equilibrium crystal symmetries in designing ferromagnetism.