Antiferroelectric Ceramics for Energy-Efficient Capacitors by Theory-Guided Discovery.

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, we apply geometric nonlinear theory of martensitic phase transitions (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. We observe a good correlation of mismatch strain with electric hysteresis, hence, with energy efficiency of AFE capacitors. Guided by theory, we conduct high-throughput materials search and discover AFE compositions with a near-perfect charge-discharge energy efficiency (98.2%), i.e., near-zero hysteresis. 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. This article is protected by copyright. All rights reserved.