$({\mathrm{Na}}_y,{\mathrm{Bi}}_z){\mathrm{Ti}}_{1-x}{\mathrm{O}}_{3(1-x)}-x{\mathrm{BaTiO}}_3$ ceramics with an excess in Bi${}^{3+}$ and/or a deficiency in Na${}^{+}$ were prepared and investigated. It is found that an antiferroelectric phase can be induced through a modulation of the mole ratio of Na${}^{+}$ and Bi${}^{3+}$. A phase boundary between ferroelectric and antiferroelectric phases can be observed at ambient temperature. A modulated phase, which is the origin of relaxor antiferroelectric behavior, should be attributed to a compositional modulation. The antiferroelectric phase can be induced to the ferroelectric phase by an applied electric field. The stability of the induced ferroelectric phase strongly depends on the mole ratio of Na${}^{+}$ and Bi${}^{3+}$. A recoverable giant strain of 0.48% comparable to PbZrO${}_3$-based antiferroelectrics as well as electrostrictive coefficients (0.026 $C^4\hspace{0.5em}{\mathrm{m}}^{-2}$) much higher than lead-based relaxor ferroelectrics with low-temperature dependence was achieved in $({\mathrm{Na}}_y,{\mathrm{Bi}}_z){\mathrm{Ti}}_{1-x}{\mathrm{O}}_{3(1-x)}-x{\mathrm{BaTiO}}_3$ antiferroelectrics. Our results show there is a high possibility that the novel lead-free antiferroelectrics will replace the PbZrO${}_3$-based ones.

• Received 10 November 2010

DOI:https://doi.org/10.1103/PhysRevB.83.054118