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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 W rec, 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 P r, 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 W rec 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.

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