| Summary: | Employing Landau theory and the Landau-Khalatnikov (L-K) equation of motion, we investigate the phase transitions in individual layers of antiferroelectric lead zirconate (PbZrO3), ferroelectric lead zirconate titanate (PbZrTiO3), and an antiferroelectric/ferroelectric PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer bulk structure. We examine the dielectric hysteresis loop behavior of the three systems, with a specific focus on the PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer under different stabilities of the PbZrO3 layer. In addition, we explore cases where the coercive field of the bilayer structure is lower than that of the PbZrTiO3 individual layer. The recoverable electric energy for the PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer increases significantly to 118 J/cm3 at an applied field of 7.5 × 108 V/m at 20 °C. In comparison, the PbZr(0.21)Ti(0.79)O3 layer reaches 71.8 J/cm3 under the same field and temperature conditions. This is much higher than those predicted experimentally by previous studies on thin film single and bilayer structures (15.6 and 28.2 J/Cm3 respectively), indicating that the antiferroelectric/ferroelectric PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer bulk structure could be used to target specific large-scale, long-term energy storage applications. Upon increasing the value of the coupling coefficient, the transition temperatures of the PbZrO3 layer and the PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer are increased up to the transition temperature of the PbZr(0.21)Ti(0.79)O3 individual layer (450 °C). This increment in the transition temperature in the bilayer system contributes to its stability in storing energy at higher temperatures. Furthermore, the recoverable energy density of the PbZrO3/PbZr(0.21)Ti(0.79)O3 bilayer increases further with temperature from 20 to 440 °C correlated with the rise in the difference between the spontaneous and the remanent polarizations (Ps − Pr). The significant stored energy observed over a wide temperature range highlights the promise of this bilayer structure for creating high-power capacitors where stability at different temperatures is crucial and possesses greater energy storage capacity. © 2024 Author(s).
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