Enhancement of Energy-Storage Density in PZT/PZO-Based Multilayer Ferroelectric Thin Films

PbZr_0.35Ti_0.65O₃ (PZT), PbZrO₃ (PZO), and PZT/PZO ferroelectric/antiferroelectric multilayer films were prepared on a Pt/Ti/SiO₂/Si substrate using the sol-gel method. Microstructures and physical properties such as the polarization behaviors, leakage current, dielectric features, and energy-storage characteristics of the three films were systematically explored. All electric field-dependent phase transitions, from sharp to diffused, can be tuned by layer structure, indicated by the polarization, shift current, and dielectric properties. The leakage current behaviors suggested that the layer structure could modulate the current mechanism, including space-charge-limited bulk conduction for single layer films and Schottky emission for multilayer thin films. The electric breakdown strength of a PZT/PZO multilayer structure can be further enhanced to 1760 kV/cm, which is higher than PZT (1162 kV/cm) and PZO (1373 kV/cm) films. A recoverable energy-storage density of 21.1 J/cm³ was received in PZT/PZO multilayers due to its high electric breakdown strength. Our results demonstrate that a multilayer structure is an effective method for enhancing energy-storage capacitors.