Influence of moisture on the ferroelectric properties of sputtered hafnium oxide thin films

While the influence of various fabrication parameters during deposition on the ferroelectricity of hafnium oxide has been extensively studied, the effect of different atmospheres on the actual switching process has not yet been investigated. In this work, we characterized the ferroelectric properties of undoped hafnium oxide prepared by reactive sputtering under three different atmospheres: dry oxygen/nitrogen, wet nitrogen, and vacuum conditions. We found a significant correlation between dry and wet atmospheres and resulting polarization. Specifically, we observed a direct effect on ferroelectric switching when the film was exposed to dry atmospheres and vacuum, resulting in a higher electric field necessary to initialize the wake-up effect due to an initial imprint effect. Increasing the amount of wet nitrogen during switching decreased the imprint and lowered the necessary voltage required for the wake up. We present a simple model that explains and discusses the incorporation of moisture and its resulting consequences on the ferroelectric properties of hafnium oxide. Additionally, kinetic Monte Carlo simulations showed that the addition of protons to the oxide thin film leads to a lowering of the potential and to a redistribution of protons and oxygen vacancies, which reduces the initial imprint.