Extrinsic scaling effects on the dielectric response of ferroelectric thin films

Abstract

Scaling effects in polycrystalline ferroelectric thin films were investigated by preparing barium titanate in a manner that maintained constant composition and film thickness while allowing systematically increased grain size and crystalline coherence. The average grain dimensions ranged from 60to110nm, and temperature dependence of permittivity analysis revealed diffuse phase transitions in all cases. Maximum permittivity values ranged from 380 to 2040 for the smallest to largest sizes, respectively. Dielectric hysteresis is evident at room temperature for all materials, indicating stability of the ferroelectric phase. Comparison of permittivity values at high electric fields indicates that the intrinsic dielectric response is identical and microstructural artifacts likely have a minimal influence on film properties across the sample series. Permittivity values, however, are substantially smaller than those reported for bulk material with similar grain dimensions. X-ray line broadening measurements were taken for the grain size series at the Cornell High Energy Synchrotron Source (CHESS), which revealed coherent scattering dimensions substantially smaller than the microscopy-determined grain size. Collectively these data sets suggest that permittivity values are influenced not only by grain size but also by the mosaic structure existing within each grain, and that thin film thermal budgets, which are several hundred degrees lower than used for bulk processing, are responsible for reduced crystalline coherence, and likely the origin of degraded electromechanical response in thin film ferroelectrics.