Design of magnetic spirals in layered perovskites: Extending the stability range far beyond room temperature

In insulating materials with ordered magnetic spiral phases, ferroelectricity can emerge owing to the breaking of inversion symmetry. This property is of both fundamental and practical interest, particularly with a view to exploiting it in low-power electronic devices. Advances toward technological applications have been hindered, however, by the relatively low ordering temperatures T_spiral of most magnetic spiral phases, which rarely exceed 100 K. We have recently established that the ordering temperature of a magnetic spiral can be increased up to 310 K by the introduction of chemical disorder. Here, we explore the design space opened up by this novel mechanism by combining it with a targeted lattice control of some magnetic interactions. In Cu-Fe layered perovskites, we obtain T_spiral values close to 400 K, comfortably far from room temperature and almost 100 K higher than using chemical disorder alone. Moreover, we reveal a linear relationship between the spiral's wave vector and the onset temperature of the spiral phase. This linear law ends at a paramagnetic-collinear-spiral triple point, which defines the highest spiral ordering temperature that can be achieved in this class of materials. On the basis of these findings, we propose a general set of rules for designing magnetic spirals in layered perovskites using external pressure, chemical substitutions, and/or epitaxial strain, which should guide future efforts to engineer magnetic spiral phases with ordering temperatures suitable for technological applications.