Ferroelastic aspects of relaxor ferroelectric behaviour in Pb(In₁/₂Nb₁/₂)O₃-Pb(Mg₁/₃Nb₂/₃)O₃-PbTiO₃ perovskite

Abstract

Elastic and anelastic properties of poled and depoled single crystals of Pb(In₁/₂Nb₁/₂)O₃-Pb(Mg₁/₃Nb₂/₃)O₃-PbTiO₃ with compositions close to the morphotropic boundary have been investigated over the temperature range 5–700 K by resonant ultrasound spectroscopy (RUS) at frequencies of 0.1–1.2 MHz. Steep elastic softening occurs in a temperature interval of at least 250 K as the Vogel-Fulcher freezing interval and cubic → tetragonal transition point, T c, are approached from above. This is understood in terms of coupling between acoustic modes and central peak mode(s) associated with dynamic polar nano regions (PNR's) below the Burns temperature. Acoustic losses occur in a temperature interval of ∼50 K above T c, associated with slowing down of the PNR dynamics. The cubic ↔ tetragonal and tetragonal ↔ rhombohedral transitions are accompanied by steep minima in elastic properties, closely analogous to the pattern of softening and stiffening observed in sequences of improper ferroelastic transitions in other perovskites. Variations in the magnitudes of acoustic losses at T < T c correlate with the density of ferroelastic twin walls, from lowest for [001]c-poled and [111]c-poled crystals in the stability fields of the tetragonal and rhombohedral phases, respectively, to highest for unpoled crystals. A simple model of Debye-like peaks in acoustic loss near 100 K has yielded activation energies and attempt frequencies in the same range as those observed from dielectric data in the Vogel-Fulcher freezing interval. These highlight the fact that, in addition to conventional ferroelectric/ferroelastic twin walls, relaxor ferroelectrics contain local structural heterogeneities coupled to strain, which are probably related to the presence of static PNR's preserved even in poled crystals. RUS also provides a convenient and effective means of determining the mechanical quality factor of relaxor ferroelectrics, as functions of both poling history and temperature.