Incommensurate modulations and thickness-dependent energy storage density in (PbLaSrBa)(ZrSnTi)O 3 relaxor antiferroelectric thick-film ceramics

In this study, (Pb0.92-xLa0.04SrxBa0.02)(Zr0.64Sn0.35Ti0.01)O3 (PLSBZSTi, i = 1 (x=0.04), 2 (0.06), 3 (0.08), and 4 (0.10)) relaxor antiferroelectric thick-film ceramics were prepared using a tape-casting process. An ultrahigh Wrec of 20.09 J/cm3 with an ultrahigh η of 91.34% was obtained for the PLSBZST2 (x = 0.06) ceramic. This outstanding energy storage performance is attributed to the distinct microstructural features of this system. Specifically, transmission electron microscopy revealed the presence of nanosized stripe domains, along with F-spots associated with 1/2{ooo} superlattice diffraction and an incommensurate modulation structure (IMS) related to the 1/n<110> superlattice (n = 4.91). These microstructural characteristics are direct evidence of oxygen octahedral tilting, which promotes the formation of relatively slim hysteresis loops. Moreover, the inverse power-law relationship between the sample thickness and energy storage density was determined. The fitted exponent was -0.43 ± 0.04, which can be quantified by combining the thickness-dependent dielectric breakdown strength (exponent of -0.39) and maximum polarization (exponent of -0.13) with a 20% correction factor accounting for the practical underutilization of the maximum electric field and polarization.