Precursor dynamics of a cubic to tetragonal ferroelectric phase transition in BaTiO3 is studied by the accurate measurement of the second harmonic generation (SHG) integral intensities. A finite signal holds for the SHG integrated intensity above the ferroelectric Curie temperature T(c)=403 K. Above the Burn's temperature T(d)≈580 K, the power law with the exponent γ=1 shows normal SHG nature originating from the hyper-Raman scattering by dynamical polar excitations, while, below T(d), a SHG signal from polar nanoregions becomes dominant with the larger exponent γ=2. Such a crossover of the power law exponent near T(d) is discussed on the basis of the effective Hamiltonian method and Monte Carlo simulation.
Raman spectra of sodium niobate (NaNbO 3 ) were obtained in all phases and revealed a significant disorder in the high-temperature U, T2 and T1 phases and a complicated folding of the Brillouin zone at the transitions into modulated S, R, P and N phases associated with the competitive zone-boundary soft modes (in-phase and out-of phase octahedral tilts) along the M-T-R line. An extensive Raman study combined with x-ray diffraction (XRD) and dielectric measurements confirmed the presence of the incommensurate (INC) phase in sodium niobate. XRD experiments revealed the invar effect in the temperature interval 410-460 K corresponding to the INC phase associated with rotations of the NbO 6 octahedra modulated along the b-direction. Our experiments suggest that the phase P consists of three phases: monoclinic (P m ) between 250 and 410 K, INC between 410 and 460 K, and orthorhombic (P o ) between 460 and 633 K. At the low-temperature transition to the ferroelectric rhombohedral N phase all folded modes originating from the M-and T-points of the Brillouin zone abruptly disappear, Raman spectra in the N phase become much simpler and all peaks were assigned.
In contrast to ordinary ferroelectrics where the temperature T m of the permittivity maximum monotonically increases with bias field E in ͑1−x͒PbMg 1/3 Nb 2/3 O 3 -͑x͒PbTiO 3 ͑0 ഛ x ഛ 0.35͒ single crystals, T m was found to remain constant or to decrease with E up to a certain threshold field E t , above which T m starts increasing. The threshold field E t decreases with increasing x, tending toward zero at approximately x = 0.4. We explain this dependence in the framework of models which take into account quenched random fields and random bonds. For crystals with 0.06ഛ x ഛ 0.13, the E-T phase diagrams are constructed. In contrast to PMN, they exhibit an additional, nearly field-independent boundary, in the vicinity of the Vogel-Fulcher temperature. We believe this boundary to correspond to an additional phase transition and the appearing order parameter is likely to be nonpolar.
In the present study, we diluted either A- or B- sublattice of perovskite multiferroic PbFe(0.5)Nb(0.5)O(3) (PFN) and studied the changes of the magnetic and ferroelectric phase transition temperatures and dielectric properties caused by such dilution. Dielectric studies of PFN single crystals show that, in contrast to the commonly adopted view, the ferroelectric phase transition in PFN is non-diffused and the relaxor-like behavior usually observed in ceramic samples has an extrinsic nature. A-site substitutions (Ba, Ca) lead to the smearing of the permittivity-temperature maximum, lowering its maximum temperature, T(m) and inducing relaxor behavior. B-site diluting of PFN by Ti increases T(m) and only slightly affects the permittivity maximum diffuseness. Both A-site and B-site substitutions in PFN lead to lowering of its Neel temperature, T(N). However, above a certain compositional threshold, fast lowering of T(N) stops and a new magnetic state with comparatively high (~50K) transition temperature becomes stable in a rather wide compositional range.
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