Elastic precursor effects during the Ba$_{1-x}$Sr$_{x}$TiO$_{3}$ ferroelastic phase transitions

TL;DR

This study investigates elastic precursor softening in Ba$_{1-x}$Sr$_{x}$TiO$_{3}$ during ferroelastic phase transitions, revealing a continuous change in behavior from displacive to order/disorder mechanisms across compositions.

Contribution

It provides a detailed analysis of the temperature evolution and nature of elastic softening, introducing a Vogel-Fulcher framework to characterize precursor effects in these materials.

Findings

Elastic softening persists up to 850 K in Ba-rich compounds.

The exponent $ppa$ varies from 1.5 in SrTiO$_{3}$ to 0.2 in BaTiO$_{3}$.

Softening remains significant (~33%) of Young's modulus at 750 K in BaTiO$_{3}$.

Abstract

Elastic softening in the paraelastic phases of Ba$_{1-x}$Sr$_{x}$TiO$_{3}$ is largest near the transition temperatures and decreases on heating smoothly over extended temperature ranges. Softening extends to the highest measured temperature(850~K) for Ba-rich compounds. The temperature evolution of the excess compliance of the precursor softening follows a power law $\delta S\propto |T-T_{\mathrm{C}}|^{-\kappa }$\ with a characteristic exponent $\kappa $\ ranging between 1.5 in SrTiO$_{3}$\ and 0.2 in BaTiO$_{3}$. The latter value is below the estimated lower bounds of displacive systems with three orthogonal soft phonon branches (0.5). An alternative Vogel-Fulcher analysis shows that the softening is described by extremely low Vogel-Fulcher energies $E_{a}$, which increase from SrTiO$_{3}$% \ to BaTiO$_{3}$\ indicating a change from a displacive to a weakly order/disorder character of the elastic precursor. Mixed crystals of Ba$_{x}$% Sr$_{1-x}$TiO$_{3}$ possess intermediate behaviour. The amplitudes of the precursor elastic softening increases continuously from SrTiO$_{3}$ to BaTiO$% _{3}$. Using power law fittings reveals that the elastic softening is still $% 33\%$ of the unsoftened Young's modulus at temperatures as high as 750 K in BaTiO$_{3}$ with $\kappa \simeq $ 0.2. This proves that the high temperature elastic properties of these materials are drastically affected by elastic precursor softening.