Enhanced Permittivity in Wurtzite ScAlN Through Nanoscale Sc Clustering

ScN alloyed AlN (Sc x Al 1‐ x N, ScAlN, or AlScN) is a wurtzite semiconductor with attractive ferroelectric, dielectric, piezoelectric, and optical properties. Here, using electron ptychography in combination with a suite of experimental and theoretical methods, we show that ScAlN films (with x spanning 0.18 to 0.36) contain nanoscale Sc‐rich clusters which maintain the wurtzite crystal structure. While both molecular beam epitaxy (MBE) and sputter deposited Sc 0.3 Al 0.7 N films show Sc clustering, the degree of clustering is significantly stronger for the MBE‐grown film, offering an explanation for some of the discrepancies between MBE‐grown and sputtered films reported in the literature. Moreover, the MBE‐grown Sc 0.3 Al 0.7 N film exhibits a dispersive and anomalously large dielectric permittivity, roughly double that of sputtered Sc 0.3 Al 0.7 N. We attribute this result to the Sc‐rich clusters locally reaching x ∼ 0.5 and approaching the predicted ferroelectric‐to‐paraelectric phase transition, resulting in a giant (local) enhancement in permittivity. The Sc‐rich clusters should similarly affect the piezoelectric, optical, and ferroelectric responses, suggesting cluster‐engineering as a means to tailor ScAlN's functional properties.