Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric

TL;DR

This study uses molecular dynamics to reveal that relaxor ferroelectrics exhibit anisotropic local correlations and a homogeneous dipole network, challenging existing models and offering new insights into their phase transitions.

Contribution

It introduces a novel model of relaxor ferroelectrics based on anisotropic local correlations and a homogeneous dipole network, supported by simulation data.

Findings

Relaxor phase characterized by anisotropic correlations between local cation displacements.

Contradicts the polar nanoregion model, proposing a homogeneous random dipole network.

Local order parameters can describe relaxor transitions.

Abstract

Relaxor ferroelectrics have been a focus of intense attention due to their anomalous dielectric characteristics, diffuse phase transitions, and strong piezoelectricity. Understanding the structure and dynamics of relaxors has been one of the long-standing challenges in solid-state physics, with the current model of polar nanoregions in a non-polar matrix providing only a qualitative description of the relaxor phase transitions. In this paper, we investigate the local structure and dynamics in 75%PbMg$_{1/3}$Nb$_{2/3}$O$_3$-25%PbTiO$_3$ (PMN-PT) using molecular dynamics simulations and the dynamic pair distribution function technique. We show for the first time that relaxor transitions can be described by local order parameters. We find that structurally, the relaxor phase is characterized by the presence of highly anisotropic correlations between the local cation displacements. These correlations resemble the hydrogen bond network in water. Our findings contradict the current polar nanoregion model; instead, we suggest a new model of a homogeneous random network of anisotropically coupled dipoles.