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Ferroelectric memories experienced a revival in the last decade due to thediscovery of ferroelectricity in HfO$_2$-based nanometer-thick thin films.These films exhibit exceptional silicon compatibility, overcoming the scalingand integration obstacles that impeded perovskite ferroelectrics' use inhigh-density integrated circuits. The exact phase responsible forferroelectricity in hafnia films remains debated with no single factoridentified that could stabilize the ferroelectric phase thermodynamically.Here, supported by density functional theory (DFT) high-throughput (HT)calculations that screen a broad range of epitaxial conditions, we demonstrateconclusively that specific epitaxial conditions achievable with commonsubstrates such as yttria-stabilized zirconia (YSZ) and SrTiO$_3$ can favor thepolar Pca2$_1$ phase thermodynamically over other polar phases such as R3m andPmn2$_1$ and nonpolar P2$_1$/c phase. The substrate's symmetryconstraint-induced shear strain is crucial for the preference of Pca2$_1$. Thestrain-stability phase diagrams resolve experiment-theory discrepancies and canguide the improvement of ferroelectric properties of epitaxial hafnia thinfilms.

Epitaxial ferroelectric hafnia stabilized by symmetry constraints