Local Polarization Heterogeneity Mediates Reversible Switching in PbZrO 3 -Based Antiferroelectrics

Abstract

Balancing high polarization, low hysteresis, and large breakdown strength remains challenging in PbZrO 3 -based antiferroelectric ceramics because of the strong coupling between longrange antipolar order and field-induced AFE-FE switching. Here, local polarization heterogeneity is regulated through moderate Sr substitution while preserving a dominant Pbam antiferroelectric framework. Atomic displacement analysis reveals locally varying correlations between antipolar and polar-like configurations, with weakly correlated transitional regions that disrupt collective switching and broaden the field-induced polarization response. The enhanced dielectric diffuseness (γ = 1.68 for x = 0.01) is consistent with the increased polarization heterogeneity. Consequently, Pb 0.97 La 0.02 Sr 0.01 (Zr 0.6 Sn 0.4 ) 0.97 Ta 0.02 O 3 achieves a recoverable energy density of 12.87 J cm -3 and an efficiency of 85.7% at 720 kV cm -1 , together with excellent cycling/frequency stability and further releasing 9.67 J cm -3 at 600 kV cm -1 within 113 ns. This work demonstrates that atomic-scale polarantipolar heterogeneity can mediate reversible switching and provide an effective route toward highperformance antiferroelectric energy-storage ceramics.