Development of “fragility” in relaxor ferroelectrics

Abstract

Relaxor ferroelectrics (RFs), a special class of the disordered crystals or ceramics, exhibit a pronounced slowdown of their dynamics upon cooling as glass-forming liquids, called the “Super-Arrhenius (SA)” relaxation. Despite great progress in glass-forming liquids, the “fragility” property of the SA relaxation in RFs remains unclear so far. By measuring the temperature-dependent dielectric relaxation in the typical relaxor Pb(Mg1/3Nb2/3)O3-x%PbTiO3 (PMN − x%PT) with 0 ≤ x ≤ 20.0, we in-depth study the “fragility” properties of the SA relaxation in PMN − x%PT. Such fascinating issues as the mechanism of the “fragility” at an atomic scale, the roles of the systematic configurational entropy change and interaction among relaxing units (RUs, including polar nanoregions and free dipoles) and the relation between “fragility” and ferroelectric order are investigated. Our results show that both the “fragility” of the temperature-dependent SA relaxation and ferroelectric order in the PMN − x%PT systems investigated arise thermodynamically from the configurational-entropy loss due to the attractive interaction among RUs, and develops as a power law, possibly diverging at the finite critical temperature Tc. A reasonable physical scenario, based on our “configurational-entropy-loss” theory and Nowick's “stress-induced-ordering” theory, was proposed.