Structural disorder differentiation regulates antiferroelectric phase stability to achieve high dielectric energy storage

Abstract

Antiferroelectric (AFE) ceramics have emerged as promising materials for high-power energy-storage applications, yet their practical performance is fundamentally constrained by the intrinsic trade-off among phase-transition stability, polarization response, and hysteresis loss. Here, we report a local disorder engineering strategy in lead zirconate titanate-based ceramics, in which Sn⁴⁺ incorporation induces a spatially heterogeneous AFE modulation that enables the simultaneous optimization of energy density and efficiency. Atomic- resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) reveals that Sn⁴⁺ partially disrupts the pristine long-range fourfold antiparallel AFE order, giving rise to the coexistence of conventional AFE domains and nanoscale microdomains with reduced displacement amplitudes and disordered polarization orientations. Phase-field simulations further demonstrate that this locally disordered AFE configuration lowers the AFE-FE phase-transition barrier and suppresses hysteresis loss, resulting in pronounced relaxor-like behavior under electric fields. As a result, the optimized (Pb_0.92Sr_0.08)(Zr_0.54Sn_0.45Ti_0.01)O₃ ceramic delivers a recoverable energy density of ∼10.49 J cm⁻³ with an efficiency of ∼87.14% at 445 kV cm⁻¹, together with a high power density of 275.9 MW cm⁻³ and an ultrafast discharge time (t_0.9) of 58.8 ns. In addition, robust thermal and frequency stability is maintained. These results demonstrate that engineering locally disordered AFE modulation provides an effective pathway for developing high-efficiency and robust energy-storage ceramics.