Abstract

Recent neutron scattering measurements performed on the relaxor ferroelectric Pb[(Zn1/3Nb2/3)0.92Ti0.08]O3 (PZN-8%PT) in its cubic phase at 500 K, have revealed an anomalous ridge of inelastic scattering centered ~0.2 A-1 from the zone center (Gehring et al., Phys. Rev. Lett. 84, 5216 (2000)). This ridge of scattering resembles a waterfall when plotted as a phonon dispersion diagram, and extends vertically from the transverse acoustic (TA) branch near 4 meV to the transverse optic (TO) branch near 9 meV. No zone center optic mode was found. We report new results from an extensive neutron scattering study of pure PZN that exhibits the same waterfall feature. We are able to model the dynamics of the waterfall using a simple coupled-mode model that assumes a strongly q-dependent optic mode linewidth Gamma1(q) that increases sharply near 0.2 A-1 as one approaches the zone center. This model was motivated by the results of Burns and Dacol in 1983, who observed the formation of a randomly-oriented local polarization in PZN at temperatures far above its ferroelectric phase transition temperature. The dramatic increase in Gamma1 is believed to occur when the wavelength of the optic mode becomes comparable to the size of the small polarized micro-regions (PMR) associated with this randomly-oriented local polarization, with the consequence that longer wavelength optic modes cannot propagate and become overdamped. Below Tc=410 K, the intensity of the waterfall diminishes. At lowest temperatures ~30 K the waterfall is absent, and we observe the recovery of a zone center transverse optic mode near 10.5 meV.

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