High AC field-induced polarization switching unraveled in frequency domain: Enhanced dielectric responses in lanthanum-doped Pb(Ni1/3Nb2/3)O3-Pb(Zr,Ti)O3 relaxor-ferroelectrics

In this study, we delve into the complex dielectric behaviors of lanthanum (La)-doped PNN-PZT relaxor-ferroelectric ceramics under the influence of high AC fields. Our approach involves a meticulous design of dielectric measurements to scrutinize the decoupling phenomenon between local polarization oscillation and global polarization switching. Remarkably, the application of high AC fields (>0.5 kV/mm) causes a dramatic increase in the dielectric permittivity (2x), alongside pronounced frequency dispersion (>65 degrees C) and a permittivity hump below T-m in 7% La-doped relaxor compositions. For relaxor-ferroelectric ceramics doped with lower La (<=5%) that are featured with tweed-like submicron domains as imaged in in situ transmission electron microscopy, the significantly enhanced dielectric permittivity and dielectric loss (>1) are induced under high AC fields (<0.5 kV/mm). A comparative study with a polarization loop in the time domain under various AC fields and DC bias demonstrates that the dielectric anomaly in the frequency domain is associated with global polarization switching, co-existing with polarization oscillation mechanism in various domains. This frequency domain method reveals threshold AC fields (0.25-0.5 kV/mm) above which polarization switching occurs in relaxor-FE compositions at elevated temperatures, complements the dynamic behaviors of P-E hysteresis, and cautions the control of AC fields in dealing with relaxor-ferroelectric materials for advanced electronic applications.