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BaTiO3-based ferroelectrics have been extensively studied due to their large dielectric constants and a high saturated polarization, which have the potential to store or supply electricity of very high energy and power densities. In order to further improve the energy efficiency η and the recyclable energy density Wrec, an A, B-site co-doped (Ba0.95,Sr0.05)(Zr0.2,Ti0.8)O3 ceramic target was used for sputter deposition of film capacitor structures on Si. This film composition reduces the remnant polarization Pr, while the choice of a low-temperature, templated sputtering process facilitates the formation of high-density arrays of columnar nanograins (average diameter d ∼20 nm) and grain boundary dead layers. This self-assembled nanostructure further delays the saturation of the electric polarization, leading to a high energy density Wrec of ∼148 J/cm3 and a high energy efficiency η of ∼90%. Moreover, the (Ba0.95,Sr0.05)(Zr0.2,Ti0.8)O3 film capacitors retain their high energy storage performance in a broad range of working temperature (-175-300 °C) and operating frequency (1 Hz-20 kHz). They are also fatigue-free after up to 2 × 109 switching cycles. Our work provides a new method and a cost-effective processing route for the creation and integration of high-performance dielectric capacitors for energy storage applications.

Dielectric capacitors have the highest charge/discharge speed among all electrical energy devices, but lag behind in energy density. Here we report dielectric ultracapacitors based on ferroelectric films of Ba(Zr0.2,Ti0.8)O3 which display high-energy densities (up to 166 J cm–3) and efficiencies (up to 96%). Different from a typical ferroelectric whose electric polarization is easily saturated, these Ba(Zr0.2,Ti0.8)O3 films display a much delayed saturation of the electric polarization, which increases continuously from nearly zero at remnant in a multipolar state, to a large value under the maximum electric field, leading to drastically improved recyclable energy densities. This is achieved by the creation of an adaptive nano-domain structure in these perovskite films via phase engineering and strain tuning. The lead-free Ba(Zr0.2,Ti0.8)O3 films also show excellent dielectric and energy storage performance over a broad frequency and temperature range. These findings may enable broader applications of dielectric capacitors in energy storage, conditioning, and conversion., Dielectric capacitors offer high-power delivery materials for energy-storage, yet suffer from low energy densities. Here, the authors prepared ferroelectric Ba(Zr0.2,Ti0.8)O3 that utilizes polydomain nanostructures to delay electric polarization saturation and boost energy densities.