Enhancing the piezoelectric activity of AlN by partially substituting Al with Sc to form Al1–xScxN is a promising approach to improve the performance of piezoelectric micro-electromechanical systems. Here, we present evidence of an instability in the morphology of Al1–xScxN, which originates at, or close to, the substrate/Al1–xScxN interface and becomes more pronounced as the Sc content is increased. Based on Transmission electron microscopy, piezoresponse force microscopy, X-ray diffraction, and SEM analysis, it is identified to be the incipient formation of (100) oriented grains. Approaches to successfully reestablish exclusive c-axis orientation up to x = 0.43 are revealed, with electrode pre-treatment and cathode-substrate distance found to exert significant influence. This allows us to present first measurements of the transversal thin film piezoelectric coefficient e31,f and dielectric loss tangent tanδ beyond x = 0.3.

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