Antiferroelectric Ceramics for Energy‐Efficient Capacitors by Theory‐Guided Discovery

Abstract Antiferroelectric ceramics, via the electric‐field‐induced antiferroelectric (AFE)–ferroelectric (FE) phase transitions, show great promise for high‐energy‐density capacitors. Yet, currently, only 70–80% energy release is found during a charge–discharge cycle. Here, for PbZrO 3 ‐based oxides, geometric nonlinear theory of martensitic phase transitions is applied (first used to guide supercompatible shape‐memory alloys) to predict the reversibility of the AFE–FE transition by using density‐functional theory to assess AFE/FE interfacial lattice‐mismatch strain that assures ultralow electric hysteresis and extended fatigue lifetime. A good correlation of mismatch strain with electric hysteresis, hence, with energy efficiency of AFE capacitors is observed. Guided by theory, high‐throughput material search is conducted and AFE compositions with a near‐perfect charge–discharge energy efficiency (98.2%), i.e., near‐zero hysteresis are discovered. And the fatigue life of the capacitor reaches 79.5 million charge–discharge cycles, a factor of 80 enhancement over AFE ceramics with large electric hysteresis.