Nanocrystalline buildup, relaxor behavior, and polarization characteristic in PZT-PNZN quaternary ferroelectrics

The Pb(Zr0.47Ti0.53)O-3-Pb[(Ni0.6Zn0.4)(1/3)Nb-2/3]O-3 (PZT-PNZN) quaternary ferroelectrics presenting the high piezoelectric coefficients are the active element in a range of piezoelectric devices. However, the buildup of nanoceramics with stable perovskite structure is still a big challenge, which prohibits the miniaturization of piezoelectric devices. In this work, the high dense PZT-PNZN nanoceramics with average grain size of 130nm were prepared by a combination of high-energy ball milling (HEBM) and spark plasma sintering (SPS). The domain configuration and relaxor behavior in this nanoceramic are reported for the first time. Although the noncubic crystal structure and dielectric anomaly suggest a ferroelectric behavior, only very slim polarization-electric (P-E) hysteresis loops are observed. The suppression of macroscopic ferroelectric polarization mainly originates from the decrease in crystal tetragonality and the enhanced clamping effect on domain wall motion. The piezoelectric properties, d(33)=65pC/N and k(p)=17%, raise the possibility of PZT-PNZN nanoceramics for application in multilayer piezoelectric devices.