Origin of high‐temperature piezoelectric stability and polar nanoregions dynamics in 0.55Bi(Mg1/2Ti1/2)O3–0.45PbTiO3

The 0.55Bi(Mg1/2Ti1/2)O3–0.45PbTiO3 ceramics exhibit notable dielectric anomalies across three temperature ranges. The low‐temperature anomaly is attributed to a reentrant dipole glass‐like relaxor behavior; the mid‐temperature anomaly results from a ferro‐paraelectric phase transition; and the high‐temperature anomaly is associated with a diffuse phase transition. The system demonstrates favorable piezoelectric, electromechanical, and ferroelectric properties. Specifically, the ceramic presents a piezoelectric coefficient (d33) of 220 pC/N, an electromechanical coupling factor (kp) of 27%, and a remanant polarization (Pr) of 32.5 μC/cm2. Moreover, it maintains an operational capability up to 643 K. The unsaturated P(E) loops are formed through the coupling polarization between polar nanoregions (PNRs) and P4mm ferroelectric domains. By examining the electrical modulus, the dynamic PNRs resulting from ferroelectric phonon localization and the formation of P4mm ferroelectric domains were analyzed. The result reveals a mesoscale coupling relationship between the origin of high‐temperature piezoelectric stability and the dynamics of PNRs, thereby providing noble insights into the (1 − x)BiMeO3–xPbTiO3 system.