NaNbO3 modulated phase transition behavior and antiferroelectric stability evolution in 0.88(Bi0.5Na0.5)TiO3-0.12BaTiO3 lead-free ceramics

Giant strains in (Bi0.5Na0.5)TiO3 based ceramics are usually attributed to electric field induced nonpolar to polar phase transition. Whether it is an ergodic relaxor R3c/P4mm ferroelectric (FE) to long-range ordered FE phase transformation or a reversible P4bm antiferroelectric (AFE) to FE phase transition is still unclear. Herein, lead-free (0.88-x)(Bi0.5Na0.5)TiO3-0.12BaTiO3-xNaNbO3 ceramics exhibit a composition-modulated FE tetragonal P4mm to relaxor AFE tetragonal P4bm phase transition, in which double hysteresis loop, sprout-shaped S-E curves, near-zero quasi-static d33 together with a large volume change suggest the AFE characteristics of P4bm phase. An interesting finding is that the reversibility of field-induced AFE P4bm phase to FE P4mm phase transition strongly depends on the NN content, from being completely irreversible at x = 0.01–0.02, to partially reversible at x = 0.03–0.05, and finally to completely reversible at x = 0.06–0.08. It is indicated that the variation of reversibility should be attributed to the change of relative free energy caused by decreasing the FE to AFE phase transition temperature with increasing the NN content.