Novel non-stoichiometric (Ba0.91Ca0.09)x(Zr0.18Ti0.82)O3 ferroelectric ceramics with improved diffuse phase transition and dielectric tunable performance

Dielectric tunable properties in ferroelectric ceramics have been optimized by a variety of approaches, e.g., isovalent/aliovalent substitution, system composite et al., while the study of non-stoichiometric regulation on the performance of BCZT ceramics was rarely concerned. Herein, a series of novel non-stoichiometric (Ba0.91Ca0.09)x (Zr0.18Ti0.82)O3 (BCZTx) ceramic specimens were successfully prepared via solid-state reaction. The microstructures of BCZTx ceramics are simultaneously investigated through XRD and SEM. The diffuse phase transition (DPT) behaviour of BCZTx ceramics are studied by the Lorentz-type empirical formula. The significant enhancement of DPT behaviour is observed at x = 1.03, which probably due to the coaction of the generation of partial Schottky defects and prominent reduction of grain size. Furthermore, a high tunability (k) 87.80%, low dielectric loss (tan delta) 0.141%, and a remarkably enhanced FOM of 623 are achieved in x = 0.99 at a low DC bias electric fields (BEFs) of 7.28 kV/cm and room temperature (RT), which is superior to that of the stoichiometric BCZT ceramics and other available reported BT-based ceramics systems in term of the dielectric tunable properties. Meanwhile, it shows that the temperature dependent CQF value of x = 0.99 remained advantageous around the RT. These findings suggested that non-stoichiometric BCZTx ceramics with x = 0.99 are significantly competitive in the applications of dielectric tunable devices at RT. The non-stoichiometric regulation is an effective approach in improving the dielectric tunability properties of BCZT ceramics.