Control of Ferroelectricity in Solution‐Processed Hafnia Films Through Annealing Atmosphere

Abstract

Chemical Solution Deposition enables low‐cost fabrication of ferroelectric HfO2 films suitable for piezoelectric applications. Control of processing parameters is of utmost importance to obtain high‐quality functional films. However, the impact of the annealing atmosphere on ferroelectric properties of solution‐processed HfO2 films is not clear. In this work, the influence of annealing atmosphere and growth methods on orientation, density and electrical properties of La:HfO2 films is studied. The 45 nm‐thick films are grown by two routes, conventional (crystallization of the final 45 nm‐thick film) and layer‐by‐layer (intermediate crystallizations of 5 nm‐thick films). Annealing is performed in N2:O2 and Ar atmosphere. Films grown by layer‐by‐layer method in an oxygen‐rich atmosphere tend to have higher density (87% of theoretical density) and remanent polarization (15 µC cm–2) than the conventional films (density and remanent polarization of 80% and 7.5 µC cm‐2). Secondary ion mass spectrometry reveals higher amounts of carbon presence in the conventional films annealed in Ar. For layer‐by‐layer films, the ability to control the preferential out‐of‐plane orientation from (111) to (002) simply by changing the annealing atmosphere, is demonstrated. The results can guide the path toward high‐quality thicker films for piezoelectric applications.