Boosting Energy-Storage in High-Entropy Pb-Free Relaxors Engineered by Local Lattice Distortion

The high-entropy strategy has shown potential in advancing the energy-storage performance of dielectric capacitors, offering benefits to a range of electronic and electrical systems. However, designing high-performance high-entropy relaxor ferroelectrics (RFEs) presents challenges due to the unclear correlation between their core effects and local polarization heterogeneity. Here, we demonstrate that by engineering the local lattice distortion, a core effect in high-entropy systems, to manipulate the local polarization configuration, a giant energy density (<i>W</i>_rec) of 18.7 J cm^-3 and high efficiency (η) of 85% can be achieved in (Bi_0.5K_0.5)TiO₃-based high-entropy bulk RFE ceramics. Atomic-level local structural analysis unveils that the local lattice distortion field can be flattened by introducing ions with less size mismatch. The increase in configurational entropy from 1.54 to 2.06R is associated with a smoother polar displacement vector field and a reduction in the size of polar clusters to several unit-cell sizes with weak coupling. Consequently, a substantial decrease in hysteresis and an enhancement in the breakdown field strength can be obtained, leading to a significant improvement in energy density by over 6 times and efficiency by 3 times. Our research establishes a relationship between local lattice distortion, atomic polar displacement, and energy-storage performance in complex high-entropy systems, providing insights for enhancing energy-storage performance via a local structure design.