Understanding the effects of electric-field-induced phase transition and polarization loop behavior on the energy storage performance of antiferroelectric PbZrO3 thin films

•Sharp antiferroelectric-ferroelectric phase transition in pulsed ablated PbZrO3 films.•Diffused antiferroelectric-ferroelectric phase transition in sol-gel PbZrO3 films.•High energy-storage performance was obtained in sol-gel PbZrO3 films.•Sol-gel PbZrO3 films exhibited high efficiency over a broad temperature range. Antiferroelectric PbZrO3 (PZO) thin-films were fabricated by pulsed laser deposition (PLD) and sol-gel techniques to investigate the effect of antiferroelectric-ferroelectric (AFE-FE) phase transition on the energy storage performance. The (100)-oriented PLD thin-films have a square-double polarization-electric field (P-E) hysteresis loop with a sharp-phase transition and the (111)-oriented sol-gel thin-films have a slanted P-E loop with a diffused-phase transition. The difference in the phase transition fields between PLD and sol-gel thin-films could be attributed to their difference in crystalline orientations. In this case, the antipolar AFE phase is along the [110]-direction of the original tetragonal-cell under zero electric-field, while the antipolar AFE phase switches into the polar FE phase under a strong enough electric-field and the tetragonal-cell becomes rhombohedral with the polar direction of [111]. Due to the larger maximum polarization and slimmer P-E loop, the higher recoverable energy-storage (Ureco) of 19.4 J/cm3 and larger energy-efficiency (η) of 70.8%, are achieved in sol-gel thin-films. More importantly, this film shows excellent charge-discharge cycling endurance of both Ureco and η values after 1010 cycles and good thermal-stability under a wide operating temperature. From the viewpoint of applications, the sol-gel method is considered to be a promising approach towards producing low-cost PZO thin-films for high-efficiency energy-storage devices over a broad temperature range.