Broad-band dielectric response of BTZ-BCT piezoceramics: soft and central mode behaviour

TL;DR

This study investigates the broad-band dielectric response of BTZ-BCT piezoceramics across a wide temperature and frequency range, revealing complex phonon and mode behaviors associated with phase transitions and polar nanoclusters.

Contribution

It provides a comprehensive analysis of soft and central mode behaviors in BTZ-BCT ceramics, linking dielectric, infrared, Raman spectra, and phase transition mechanisms.

Findings

Soft phonon softens with cooling but becomes temperature independent below 500 K.

A central mode activates in terahertz and microwave spectra, driving phase transitions.

Polar nanoclusters are evidenced by Raman spectra showing new phonons above T$_{C1}$.

Abstract

Dielectric properties of BTZ-BCT ceramics were probed in the frequency range from 10 Hz to 100 THz in a broad temperature range (10-900 K). Polar soft phonon observed in infrared spectra softens with cooling, however below 500 K its frequency becomes temperature independent. Simultaneously, a central mode activates in terahertz and microwave spectra; and it actually drives the ferroelectric phase transitions. Consequently, the phase transition strongly resemble a crossover between the dispacive and order-disorder type. The central mode vanishes below 200 K. The dielectric relaxation in the radiofrequency and microwave range anomalously broadens on cooling below T$_{C1}$ resulting in the nearly frequency independent dielectric loss bleow 200 K. This broadening comes from a broad frequency distribution of ferroelectric domain wall vibrations. Raman spectra reveal new phonons below 400 K, i.e. already 15 K above T$_{C1}$. Several weak modes are detected in the paraelectric phase up to 500 K in the Raman spectra. Activation of these modes is ascribed to the presence of polar nanoclusters in the material.