Supercritical Relaxor Nanograined Ferroelectrics for Ultrahigh-Energy-Storage Capacitors

Supercritical relaxor nanograined ferroelectrics are demonstrated for high-performance dielectric capacitors, showing record-high overall properties of energy density ≈13.1 J cm−3 and field-insensitive efficiency ≈90% at ≈74 kV mm−1 and superior charge–discharge performances of high power density ≈700 MW cm−3, high discharge energy density ≈6.67 J cm−3, and ultrashort discharge time <40 ns at 55 kV mm−1. Ex/in situ transmission electron microscopy, Raman spectroscopy, and synchrotron X-ray diffraction provide clear evidence of the supercritical behavior in (Na,K)(Sb,Nb)O3–SrZrO3–(Bi0.5Na0.5)ZrO3 ceramics, being achieved by engineering the coexistence of multiple local symmetries within the ergodic relaxor zone. The vanished difference between the ground relaxor state and the high-field supercritical state eliminates polarization hysteresis. The supercritical evolution with electric field enables a highly delayed polarization saturation with continuously increased polarization magnitudes. The results demonstrate that such a design strategy of compositionally induced and field-manipulated supercritical behavior can be generalizable for developing desirable energy-storage dielectrics for applications in ceramic/film capacitors.