Central mode and soft mode behavior in PbMg1/Nb2/3O3 relaxor ferroelectric

TL;DR

This study investigates the dielectric and vibrational properties of PbMg1/Nb2/3O3 relaxor ferroelectric films, revealing the behavior of soft and central modes across a wide temperature range and their relation to polar nanoclusters.

Contribution

It provides new insights into the soft mode dynamics and the central mode behavior in PbMg1/Nb2/3O3, highlighting differences between thin film and bulk relaxors and discussing mode damping discrepancies.

Findings

Soft mode follows Cochran law with Burns temperature at 670 K.

Central mode slows down dramatically below room temperature.

A new heavily damped mode appears in FTIR spectra at low temperatures.

Abstract

The relaxor ferroelectric PbMg1/Nb2/3O3 was investigated by means of broad-band dielectric and Fourier Transform Infrared (FTIR) transmission spectroscopy in the frequency range from 1 MHz to 15 THz at temperatures between 20 and 900 K using PMN films on infrared transparent sapphire substrates. While thin film relaxors display reduced dielectric permittivity at low frequencies, their high frequency intrinsic or lattice response is shown to be the same as single crystal/ceramic specemins. It was observed that in contrast to the results of inelastic neutron scattering, the optic soft mode was underdamped at all temperatures. On heating, the TO1 soft phonon followed the Cochran law with an extrapolated critical temperature equal to the Burns temperature of 670 K and softened down to 50 cm-1. Above 450 K the soft mode frequency leveled off and slightly increased above the Burns temperature. A central mode, describing the dynamics of polar nanoclusters appeared below the Burns temperature at frequencies near the optic soft mode and dramatically slowed down below 1 MHz on cooling below room temperature. It broadened on cooling, giving rise to frequency independent losses in microwave and lower frequency range below the freezing temperature of 200 K. In addition, a new heavily damped mode appeared in the FTIR spectra below the soft mode frequency at room temperature and below. The origin of this mode as well as the discrepancy between the soft mode damping in neutron and infrared spectra is discussed.