Gradient Strain‐Induced Room‐Temperature Ferroelectricity in Magnetic Double‐Perovskite Superlattices

Abstract Single‐phase multiferroics suffer from a fundamental contradiction between polarity and magnetism in d0 electronic configuration, motivating studies of unconventional ferroelectricity in magnetic oxides. However, low critical temperature and polarization still need to be overcome. Here, it is reported that the switchable polarization behavior at room temperature in [(La2NiMnO6)/(La2CoMnO6)]n double‐perovskite magnetic superlattice films is achieved by engineering a microstructure with gradient strains, and the ferromagnetic Curie temperature did not show a rapid decrease. The synergy of gradient strains and superlattice components plays a decisive role in inducing ferroelectricity via the tilting or rotation of various oxygen octahedra. Such distortion responses to gradient strains are accompanied by slight magnetic fluctuations, maximizing the preservation of the initial magnetic exchange interactions, which alleviates the contradiction of multiferroic coexistence to a certain extent. This work confirms the room‐temperature ferroelectricity in double‐perovskite superlattices and provides a preferred strategy for confronting the difficulty of multiferroic coexistence in single‐phase materials.