Connecting the Multiscale Structure with Macroscopic Response of Relaxor Ferroelectrics

Abstract

Abstract Lead‐based relaxor ferroelectrics are characterized by outstanding piezoelectric and dielectric properties, making them useful in a wide range of applications. Despite the numerous models proposed to describe the relation between their nanoscale polar structure and the large properties, the multiple contributions to these properties are not yet revealed. Here, by combining atomistic and mesoscopic‐scale structural analyses with macroscopic piezoelectric and dielectric measurements across the (100– x )Pb(Mg 1/3 Nb 2/3 )O 3 – x PbTiO 3 (PMN– x PT) phase diagram, a direct link is established between the multiscale structure and the large nonlinear macroscopic response observed in the monoclinic PMN‐ x PT compositions. The approach reveals a previously unrecognized softening effect, which is common to Pb‐based relaxor ferroelectrics and arises from the displacements of low‐angle nanodomain walls, facilitated by the nanoscale polar character and lattice strain disorder. This comprehensive comparative study points to the multiple, distinct mechanisms that are responsible for the large piezoelectric response in relaxor ferroelectrics.