Symmetry-informed design of magnetoelectric coupling in the manganite perovskite CeBaMn2O6†

Magnetoelectric multiferroics hold great promise for the development of new sustainable memory devices. However, practical applications of many existing multiferroic materials are infeasible due to the weak nature of the coupling between the magnetic and electrical orderings, meaning new magnetoelectric multiferroics featuring intrinsic coupling between their component orderings are sought instead. Here, we apply a symmetry-informed design approach to identify and realize the new manganite perovskite CeBaMn₂O₆ in which magnetoelectric coupling can be achieved via an intermediary non-polar structural distortion. Through first-principles calculations, we demonstrate that our chosen prototype system contains the required ingredients to achieve the desired magnetoelectric coupling. Using high-pressure/high-temperature synthesis conditions, we have been able to synthesize the CeBaMn₂O₆ perovskite system for the first time. Our subsequent neutron and electron diffraction measurements reveal that the desired symmetry-breaking ingredients exist in this system on a nanoscopic length scale, enabling magnetoelectric nanoregions to emerge within the material. Through this work, we showcase the potential of the new CeBaMn₂O₆ perovskite material as a promising system in which to realize strong magnetoelectric coupling, highlighting the potential of our symmetry-informed design approach in the pursuit of new magnetoelectric multiferroics for next-generation memory devices.