Multiferroic nitride perovskites with giant polarizations and large magnetic moments

Multiferroics with coupling between ferroelectricity and magnetism have been pursued for decades. However, their magnetoelectric performances remain limited due to the common trade-off between ferroelectricity and magnetism. Here, a family of nitride perovskites is proposed as multiferroics with prominent physical properties and nontrivial mechanisms. Taking GdWN${}_3$ as a prototype, our first-principles calculations found that its perovskite phases own large polarizations (e.g. $111.3$ $\mu$C/cm${}^2$ for the $R3c$ phase) and a magnetic moment $7$ ${\mu }_{\mathrm{B}}$/Gd${}^{3+}$. More interestingly, its ferroelectric origin is multiple, with significant contributions from both Gd${}^{3+}$ and W${}^{6+}$ ions, different from its sister member LaWN${}_3$ in which the ferroelectricity almost arises from W${}^{6+}$ ions only. With decreasing size of rare earth ions, the A site ions would contribute more and more to the ferroelectric instability. Considering that small rare earth ions can be primary origins of both proper ferroelectricity and magnetism in nitride perovskites, our work provides a route to pursuit more multiferroics with unconventional mechanisms and optimal performances.