Supercritical Relaxor Nanograined Ferroelectrics for Ultrahigh‐Energy‐Storage Capacitors

Abstract

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 -(Bi_0.5 Na_0.5 )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.