From Prediction to Experimental Realization of Ferroelectric Wurtzite Al$_{1-x}$Gd$_{x}$N Alloys

AlN-based alloys find widespread application in high-power microelectronics, optoelectronics, and electromechanics. The realization of ferroelectricity in wurtzite AlN-based heterostructural alloys has opened up the possibility of directly integrating ferroelectrics with conventional microelectronics based on tetrahedral semiconductors such as Si, SiC and III-Vs, enabling compute-in-memory architectures, high-density data storage, and more. The discovery of AlN-based wurtzite ferroelectrics has been driven to date by chemical intuition and empirical explorations. Here, we demonstrate the computationally-guided discovery and experimental demonstration of new ferroelectric wurtzite Al$_{1-x}$Gd$_x$N alloys. First-principles calculations indicate that the minimum energy pathway for switching changes from a collective to an individual switching process with a lower overall energy barrier, at a rare-earth fraction $x$ of $x>$ 0.10$-$0.15. Experimentally, ferroelectric switching is observed at room temperature in Al$_{1-x}$Gd$_x$N films with $x>$ 0.12, which strongly supports the switching mechanisms in wurtzite ferroelectrics proposed previously (Lee et al., $\textit{Science Advances}$ 10, eadl0848, 2024). This is also the first demonstration of ferroelectricity in an AlN-based alloy with a magnetic rare-earth element, which could pave the way for additional functionalities such as multiferroicity and opto-ferroelectricity in this exciting class of AlN-based materials.