Polarization configuration engineering by compositional and structural tuning in piezoelectrics holds great promise for high piezoelectricity that benefits wide electromechanical applications. Here, a novel flexible polarization configuration is achieved in high-entropy Pb-based perovskites, which contributes to superior piezoelectricity of d₃₃ ∼1200 pC/N. Emergent characteristics and behaviors of such a flexible polarization configuration are thoroughly investigated by the combination of atomic-scale scanning transmission electron microscopy, in-situ high-energy synchrotron X-ray diffraction, and first-principles calculations. The multiple interactions among the A and B-site atoms, originating from the increase of the species of B-site elements as well as the enhanced entropy of the system, weaken the long-range polarization order, enhance the flexibility of the polarization under the external field, and eventually result in the high piezoelectric performance. This work demonstrates that polarization configuration engineering through the high-entropy method would be an effective strategy for obtaining outstanding piezoelectric properties, which provides new opportunities for the design and discovery of high-performance piezoelectrics.

通过压电材料中的成分和结构调谐进行极化配置工程为高压电性带来了巨大的希望，这有利于广泛的机电应用。在这里，在高熵 Pb 基钙钛矿中实现了一种新颖的柔性极化配置，这有助于d ₃₃ ∼1200 pC/N 的优异压电性。通过结合原子尺度扫描透射电子显微镜、原位高能同步辐射 X 射线衍射和第一性原理计算，彻底研究了这种灵活偏振配置的出现特性和行为。A和B之间的多重相互作用位原子，源于B位元素种类的增加以及系统熵的增强，削弱了长程极化顺序，增强了外场下极化的灵活性，最终导致高压电性能。这项工作表明，通过高熵方法进行极化配置工程将是获得优异压电性能的有效策略，这为高性能压电的设计和发现提供了新的机会。