Abstract
The relationships linking temperature and voltage dependent dielectric response, grain size, and thermal budget during synthesis are illustrated. In doing so, it was found that maximizing thermal budgets within experimental bounds leads to electrical properties comparable to the best literature reports irrespective of the processing technique or microstructure. The optimal film properties include a bulk transition temperature, a room temperature permittivity of 1800, a voltage tuning ratio of 10:1 at 450 kV/cm, and a loss tangent less than 1.5% at 450 kV/cm. The sample set illustrates the well-known relationship between permittivity and crystal dimension, and the onset of a transition temperature shifts at very fine grain sizes. A brick wall model incorporating a high permittivity grain and a low permittivity grain boundary is used to interpret the dielectric data. However, the data show that high permittivity and tunability values can be achieved at grain sizes or film thicknesses that many reports associate with dramatic reductions in the dielectric response. These differences are discussed in terms of crystal quality and maximum processing temperature. The results collectively suggest that scaling effects in ferroelectric thin films are in many cases the result of low thermal budgets and the consequently high degree of structural imperfection and are not from the existence of low permittivity phases at the dielectric-electrode interface.
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