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Raman scattering experiments on stoichiometric, Mott-insulating LaTiO_{3} over a wide range of excitation energies reveal a broad electronic continuum which is featureless in the paramagnetic state, but develops a gap of ~800 cm^{-1} upon cooling below the Néel temperature T_{N}=146 K. In the antiferromagnetic state, the spectral weight below the gap is transferred to well-defined spectral features due to spin and orbital excitations. Low-energy phonons exhibit pronounced Fano anomalies indicative of strong interaction with the electron system for T>T_{N}, but become sharp and symmetric for T
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We investigate the interplay of magnetization and lattice vibrations in rare-earth orthoferrites RFeO3, with a specific focus on non-symmetry-breaking anomalies. To do so, we study the magnetization, magnon excitations and lattice dynamics as a function of temperature in NdFeO3, TbFeO3, EuFeO3 and GdFeO3. The magnetization shows distinct temperature anomalous behavior for all investigated rare-earth orthoferrites, even in the compounds with no phase transitions occurring at those temperatures. Through spin-phonon coupling, these magnetic changes are mirrored by the FeO6 rotation mode for all the studied RFeO3, revealing a common magnetostructural effect associated with the octahedra rotations. The R3+ oscillation modes evidence a Fe3+/R3+ spins cross-talk for the NdFeO3 and TbFeO3 cases. Our work sheds light into the common magnetostructural coupling in rare-earth orthoferrites, and the important role of magnetic anisotropy and spin-orbit coupling strength of the R-Fe interactions on the spin-reorientation transition at high temperatures.
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Recent studies carried out with atomic force microscopy or high-resolution transmission electron microscopy reveal that ferroic domain walls can exhibit different physical properties than the bulk of the domains, such as enhanced conductivity in insulators, or polar properties in non-polar materials. In this review we show that optical techniques, in spite of the diffraction limit, also provide key insights into the structure and physical properties of ferroelectric and ferroelastic domain walls. We give an overview of the uses, specificities and limits of these techniques, and emphasize the properties of the domain walls that they can probe. We then highlight some open questions of the physics of domain walls that could benefit from their use.
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Ferroic domain walls are currently investigated by several state-of-the art techniques in order to get a better understanding of their distinct, functional properties. Here, principal component analysis (PCA) of Raman maps is used to study ferroelectric domain walls (DWs) in LiNbO3 and ferroelastic DWs in NdGaO3. It is shown that PCA allows us to quickly and reliably identify small Raman peak variations at ferroelectric DWs and that the value of a peak shift can be deduced-accurately and without a priori-from a first order Taylor expansion of the spectra. The ability of PCA to separate the contribution of ferroelastic domains and DWs to Raman spectra is emphasized. More generally, our results provide a novel route for the statistical analysis of any property mapped across a DW.
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The understanding of domain structures, specifically domain walls, currently attracts a significant attention in the field of (multi)-ferroic materials. In this article, we analyze contrast formation in full field electron microscopy applied to domains and domain walls in the uniaxial ferroelectric lithium niobate, which presents a large 3.8 eV band gap and for which conductive domain walls have been reported. We show that the transition from Mirror Electron Microscopy (MEM - electrons reflected) to Low Energy Electron Microscopy (LEEM - electrons backscattered) gives rise to a robust contrast between domains with upwards (Pup) and downwards (Pdown) polarization, and provides a measure of the difference in surface potential between the domains. We demonstrate that out-of-focus conditions of imaging produce contrast inversion, due to image distortion induced by charged surfaces, and also carry information on the polarization direction in the domains. Finally, we show that the intensity profile at domain walls provides experimental evidence for a local stray, lateral electric field.
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The ferroelectric phase transition in a semiconductor Sn(2)P(2)S(6) single crystal has been studied by means of high-resolution synchrotron x-ray diffraction in the pressure-temperature range where an incommensurate modulated phase has been anticipated for many years. In contrast with the predictions, the present measurements reveal only a direct ferroelectric-paraelectric phase transition close to T = 100 K, p = 1.1 GPa. In the vicinity of this phase transition, a characteristic critical diffuse scattering was observed, but no satellite peaks could be resolved there. It is concluded that the earlier hypothesis about the presence of an incommensurate phase and associated Lifshitz point in the temperature-pressure phase diagram of Sn(2)P(2)S(6) is incorrect.
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High pressure measurements of the ferroelastic phase transition of SrTiO3 (Guennou et al 2010 Phys. Rev. B 81 054115) showed a linear pressure dependence of the transition temperature between the cubic and tetragonal phase. Furthermore, the pressure induced transition becomes second order while the temperature dependent transition is near a tricritical point. The phase transition mechanism is characterized by the elongation and tilt of the TiO6 octahedra in the tetragonal phase, which leads to strongly nonlinear couplings between the structural order parameter, the volume strain and the applied pressure. The phase diagram is derived from the Clausius-Clapeyron relationship and is directly related to a pressure dependent Landau potential. The nonlinearities of the pressure dependent strains lead to an increase of the fourth order Landau coefficient with increasing pressure and, hence, to a tricritical-second order crossover. This behaviour is reminiscent of the doping related crossover in isostructural KMnF3.
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Raman scattering is used to observe pronounced electronic excitations around 230 meV--well above the two-phonon range--in the Mott insulators LaTiO3 and YTiO3. Based on the temperature, polarization, and photon energy dependence, the modes are identified as orbital excitations. The observed profiles bear a striking resemblance to magnetic Raman modes in the insulating parent compounds of the superconducting cuprates, indicating an unanticipated universality of the electronic excitations in transition metal oxides.