Dielectric relaxation and polar phonon softening in relaxor ferroelectric PbMg1/3Ta2/3O3

Relaxor ferroelectric PbMg1/3Ta2/3O3 ceramics and thin films were investigated by means of broad-band dielectric, time-domain terahertz (THz), and Fourier-transform infrared (IR) spectroscopy in the frequency range 100 Hz-90 THz at temperatures 100-490 K; the THz and IR spectra were studied from 20 to 900 K. A diffused and strongly temperature dependent peak in the complex permittivity is caused by a dielectric relaxation due to the dynamics of polar clusters. The relaxation appears below the Burns temperature T-d in the THz range; it slows down on cooling through the microwave and MHz range and anomalously broadens. The shortest and longest relaxation times of the distribution of relaxation times follow Arrhenius and Vogel-Fulcher laws, respectively. The degree of the B-site order has only a small influence on the parameters of the dielectric relaxation and almost no influence on the phonon parameters. Below T-m congruent to 180 K the distribution of relaxation frequencies becomes broader than our experimental spectral range, and frequency independent dielectric losses develop below 100 GHz in the spectra. Although the macroscopic crystal structure is cubic, IR spectra give evidence about the lower local symmetry, which can be assigned to the presence of the polar clusters below T-d. Infrared spectra above T-d still reveal more modes than predicted by selection rules in the paraelectric phase of the Fm (3) over barm space group so that we suggest selection rules which take into account chemical inhomogeneity in the beta"-perovskite sublattice. (C) 2007 American Institute of Physics.