Environmentally
friendly lead-free piezoelectric materials have
been attracting significant attention in recent years. Na1/2Bi1/2TiO3-based relaxor ferroelectrics have
found acceptance for application in promising lead-free transducers
in high-power ultrasonic devices. However, their low thermal stability,
i.e., their relatively low ferroelectric-relaxor transition temperature
(T
F‑R), hinders their practical
application. Herein, a thermal-quenching approach is applied on a
Na1/2Bi1/2TiO3 (NBT)-based single
crystal, which yields a large increase in T
F‑R and dramatic enhancement of its ferroelectric ordering, leading
to excellent thermal stability of its dielectric, ferroelectric, and
piezoelectric properties. This behavior is mainly attributed to quenching-induced
domain evolution as well as its octahedral tilt, which is linked to
the increased oxygen vacancies. The substitution of long-range ordered
ferroelectric domains for short-range polar nanodomains contributes
to its increased coherence length and, consequently, enhancement of T
F‑R. This work provides an approach to
the optimization of the ferroelectric ordering and thermal stability
of NBT as well as an in-depth understanding of the quenching effect
on the local structure, which could be applied to other relaxor-based
ferroelectrics for optimization of their macroscopic properties.