Enhanced energy storage in antiferroelectrics via antipolar frustration.

Dielectric-based energy storage capacitors characterized with fast charging and discharging speed and reliability play a vital role in cutting-edge electrical and electronic equipment. In pursuit of capacitor miniaturization and integration, dielectrics must offer high energy density and efficiency. Antiferroelectrics with antiparallel dipole configurations have been of significant interest for high-performance energy storage due to their negligible remanent polarization and high maximum polarization in the field-induced ferroelectric state. However, the low antiferroelectric-ferroelectric phase-transition field and accompanying large hysteresis loss deteriorate energy density and reliability. Here, guided by phase-field simulations, we propose a new strategy to frustrate antipolar ordering in antiferroelectrics by incorporating non-polar or polar components. Our experiments demonstrate that this approach effectively tunes the antiferroelectric-ferroelectric phase-transition fields and simultaneously reduces hysteresis loss. In PbZrO-based films, we hence realized a record high energy density among all antiferroelectrics of 189 J cm along with a high efficiency of 81% at an electric field of 5.51 MV cm, which rivals the most state-of-the-art energy storage dielectrics. Atomic-scale characterization by scanning transmission electron microscopy directly revealed that the dispersed non-polar regions frustrate the long-range antipolar ordering, which contributes to the improved performance. This strategy presents new opportunities to manipulate polarization profiles and enhance energy storage performances in antiferroelectrics.