Breaking the Energy Storage Trade-off in Antiferroelectrics via Bi³⁺-Driven Atomic-Nanoscale Synergy

Achieving superior energy storage in antiferroelectric ceramics is limited by a fundamental compromise: realxor behavior comes at the cost of sacrificing polarization strength. This directly leads to a mutually restrictive balance between recoverable energy density (W_rec) and energy storage efficiency (η). To overcome this, we develop a Bi-induced local bonding modulation strategy in Pb_0.92-1.5xSr_0.08Bi_xZr_0.49Sn_0.5Ti_0.01O₃ ceramics that simultaneously strengthens the AFE framework and refines polarization response. This approach elevates both the breakdown strength and the AFE-FE transition field, allowing the material to withstand higher electric fields and release greater stored energy. The optimized composition achieves a record-high W_rec of 15.6 J cm⁻³ with ∼90% efficiency under 600 kV cm⁻¹, alongside ultrafast discharge (t_0.9 ∼64.5 ns) and excellent thermal/frequency stability. Atomic-scale characterization reveals a coexistence of robust long-range AFE order and local polar heterogeneity, which collectively smooths the field-induced transition path and suppresses early breakdown. This work provides a generalizable design principle for dielectric capacitors by strategically decoupling polarization enhancement from relaxor behavior, paving the way for high-energy, high-efficiency pulsed-power systems.