X-ray diffraction, dynamical mechanical analysis and infrared reflectivity studies revealed an antiferrodistortive phase transition in EuTiO3 ceramics. Near 300K the perovskite structure changes from cubic Pm-3m to tetragonal I4/mcm due to antiphase tilting of oxygen octahedra along the c axis (a0a0c- in Glazer notation). The phase transition is analogous to SrTiO3. However, some ceramics as well as single crystals of EuTiO3 show different infrared reflectivity spectra bringing evidence of a different crystal structure. In such samples electron diffraction revealed an incommensurate tetragonal structure with modulation wavevector q ~ 0.38 a*. Extra phonons in samples with modulated structure are activated in the IR spectra due to folding of the Brillouin zone. We propose that defects like Eu3+ and oxygen vacancies strongly influence the temperature of the phase transition to antiferrodistortive phase as well as the tendency to incommensurate modulation in EuTiO3.Comment: PRB, in pres
Polarized Raman, IR and time-domain THz spectroscopy of orthorhombic lead zirconate single crystals yielded a comprehensive picture of temperature-dependent quasiharmonic frequencies of its low-frequency phonon modes. It is argued that these modes primarily involve vibration of Pb and/or oxygen octahedra librations and their relation to particular phonon modes of the parent cubic phase is proposed. Counts of the observed IR and Raman active modes belonging to distinct irreducible representations agree quite well with group-theory predictions. The most remarkable finding is the considerably enhanced frequency renormalization of the y-polarized polar modes, resulting in a pronounced low temperature dielectric anisotropy. Results are discussed in terms of contemporary phenomenological theory of antiferroelectricity.PACS numbers: 77.80.Bh, 77.84.Cg Although the ferroelectric and antiferroelectric materials have a lot in common, the latter have been much less investigated. An obvious reason is the absence of the direct linear coupling of the antiferroelectric (AF) order parameter to the macroscopic electric field.At the same time, a nonlinear coupling to the macroscopic electric field is still present. Therefore, AF materials actually do provide interesting functionalities, as well. In fact, the AF oxides are promising materials for high-energy storage capacitors, high-strain actuators and perhaps even for electrocaloric refrigerators [1][2][3]. The interest in the improvement of our understanding of AF oxides has been expressed recently [1,2,4,5].Lead zirconate, PbZrO 3 , is the best known example of an AF oxide -it is an end-member of technologically relevant solid solutions with PbTiO 3 (piezoelectric PZTs) [1,2,4,[6][7][8]. The parent paraelectric phase is a simple cubic perovskite with a 5-atom unit cell (P m3m, Z=1). Below the AF phase transition (T C ∼ 500 K), it goes over into an orthorhombic P bam (Z=8) structure [10,11]. The space-group symmetry change can be well understood[1] as a result of the condensation of two order parameters [1,4,9,12]. One of them is a polarization wave of a propagation vector Q Σ = (0.25, 0.25, 0) pc , the other order parameter is a Q R = (0.5, 0.5, 0.5) pc oxygen octahedra tilt mode (here pc stands for pseudocubic lattice, see Figs. 1-2).Superpositions of Q Σ , Q R include also Γ, X, M and Q S = (0.25, 0.25, 0.5) pc cubic-phase Brillouin zone points. All of these points become Brillouin zone centers in the P bam phase (see Fig. 2). Nevertheless, recent inelastic X-ray scattering experiments [4] have clearly demonstrated that the critical scattering occurs only in the vicinity of the Γ-point. Based on this experimental result, it was proposed that the AF phase transition is driven by a single mode, the Γ-point ferroelectric soft mode [4]. Within this model, the condensation of the Q Σ -point mode can be ascribed to the flexoelectric coupling with the ferroelectric mode, and the condensation of the Q R -point mode can be explained as due to a biquadratic coupling with the Q Σ m...
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