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Large magnetoelectric response in thin films is highly desired forhigh-throughput and high-density microelectronic applications. However, the d0rule in single-phase compounds usually results in a weak interaction betweenferroelectric and magnetic orders; the magnetoelectric coupling via elasticresonance in composites restricts their thin-film integration in broadband.Here, we effectuate a concurrence of ferroelectric-like and antiferromagneticphase transitions in Sr2IrO4/SrTiO3 superlattices by artificial designperiodically non-equivalent interfaces, where a maximum magnetoelectriccoefficient of ~980 mV cm-1 Oe-1 can be measured. Evidenced by synchrotronX-ray absorption and electron energy loss spectroscopies, a lopsided electronoccupation occurs at the interfacial Ti ions. From perturbative calculationsand numerical results, a strong coupling of antiferromagnetism and asymmetricelectron occupation mediated by spin-orbit interaction leads to a large bulkmagnetoelectric response. This atomic tailoring of the quantum order parametersin 3d and 5d oxides provides an alternative pathway towards strongmagnetoelectric effects with thin-film integrations.

Large Magnetoelectric Response in Sr2IrO4/SrTiO3 superlattices with non-equivalent interfaces