Polarized Raman study of the phonon dynamics in Pb(Mg$_{1/3}$Nb$%_{2/3} $)O$_{3}$ crystal

TL;DR

This study uses polarized Raman spectroscopy to analyze phonon dynamics and structural transformations in Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$, revealing how ion displacements and disorder influence relaxor behavior across temperatures.

Contribution

It provides a detailed model linking ion off-centering, reorientational motion, and spectral features in lead relaxor ferroelectrics, advancing understanding of their microscopic mechanisms.

Findings

Formation of Fm3m symmetry in ordered regions.

Reorientation of ions reduces from eight to one site with decreasing temperature.

Raman scattering results from multiphonon interactions mediated by disorder.

Abstract

Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ is one of the simplest representatives of the class of lead relaxors and often serves as a model system for more complicated compounds. In this paper we analyse both polarized and depolarized Raman scattering spectra, measured in the temperature range between 1000 and 100 K, by multiple peak decomposition. Basing on this analysis, we present the picture of transformations in the crystal and the nature of the spectral lines. According to our model, the formation of the Fm3m symmetry in the chemically ordered regions as well as the appearance and freezing of the polar nanoregions are the consequences of the same phenomenon: ion off-centered displacements and their reorientational thermal motion. The lowering temperature progressively limits this motion from eight to four, two and only one site. Raman scattering exists due to the presence of the Fm3m and polar clusters. It is a product of the multiphonon interaction process, mediated by the presence of the dynamic and static disorder.