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Register a new userColossal Spin-Phonon Anomalies and the Ferroelectric Phase Transition in the Model Multiferroic Bifeo3
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We report a temperature-dependent Raman and neutron scattering investigation of the multiferroic material bismuth ferrite BiFeO3 (BFO).
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A prominent band centered at around 1000-1300 cm-1 and associated with resonant enhancement of two-phonon Raman scattering is reported in multiferroic BiFeO3 thin films and single crystals. A strong anomaly in this band occurs at the antiferromagnetic Neel temperature. This band is composed of three peaks, assigned to 2A4, 2E8, and 2E9 Raman modes. While all three peaks were found to be sensitive to the antiferromagnetic phase transition, the 2E8 mode, in particular, nearly disappears at TN on heating, indicating a strong spin-two phonon coupling in BiFeO3.
In multiferroic BiFeO3 thin films grown on highly mismatched LaAlO3 substrates, we reveal the coexistence of two differently distorted polymorphs that leads to striking features in the temperature dependence of the structural and multiferroic properties. Notably, the highly distorted phase quasi-concomitantly presents an abrupt structural change, transforms from a hard to a soft ferroelectric and transitions from antiferromagnetic to paramagnetic at 360+/-20 K. These coupled ferroic transitions just above room temperature hold promises of giant piezoelectric, magnetoelectric and piezomagnetic responses, with potential in many applications fields.
We have carried out temperature-dependent inelastic neutron scattering measurements of YMnO3 over the temperature range 50 - 1303 K, covering both the antiferromagnetic to paramagnetic transition (70 K), as well as the ferroelectric to paraelectric transition (1258 K). Measurements are accompanied by first principles calculations of phonon spectra for the sake of interpretation and analysis of the measured phonon spectra in the room temperature ferroelectric (P63cm) and high temperature paraelectric (P63/mmc) hexagonal phases of YMnO3. The comparison of the experimental and first-principles calculated phonon spectra highlight unambiguously a spin-phonon coupling character in YMnO3. This is further supported by the pronounced differences in the magnetic and non-magnetic phonon calculations. The calculated atomistic partial phonon contributions of the Y and Mn atoms are not affected by inclusion of magnetic interactions, whereas the dynamical contribution of the O atoms is found tochange. This highlights the role of the super-exchange interactions between the magnetic Mn cations, mediated by O bridges. Phonon dispersion relations have also been calculated, in the entire Brillouin zone, for both the hexagonal phases. In the high-temperature phase, unstable phonon mode at the K point is highlighted. The displacement pattern at the K-point indicates that the freezing of this mode along with the stable mode at the {Gamma}-point may lead to a stabilization of the low-temperature (P63cm) phase, and inducing ferroelectricity. Further, we have also estimated the mode Gruneisen parameter and volume thermal expansion behavior. The latter is found to agree with the available experimental data.
The ZFC and FC magnetization dependence on temperature was measured for BiFeO3 ceramics at the applied magnetic field up to H=10T in 2K-1000K range. The antiferromagnetic order was detected from the hysteresis loops below the Neel temperature TN=646K. In the low magnetic field range there is an anomaly in M(H), probably due to the field-induced transition from circular cycloid to the anharmonic cycloid. At high field limit we observe the field-induced transition to the homogeneous spin order. From the M(H) dependence we deduce that above the field Ha the spin cycloid becomes anharmonic which causes nonlinear magnetization, and above the field Hc the cycloid vanishes and the system again exhibits linear magnetization M(H). The anomalies in the electric properties, which are manifested within the 640K-680K range, coincide to the anomaly in the magnetization M(T) dependence, which occurs in the vicinity of TN. We propose to ascribe this coincidence to the critical behaviour of the chemical potential, related to the magnetic phase transition.
We discuss the first infrared reflectivity measurement on a BiFeO3 single crystal between 5 K and room temperature. The 9 predicted ab-plane E phonon modes are fully and unambiguously determined. The frequencies of the 4 A1 c-axis phonons are found. These results settle issues between theory and data on ceramics. Our findings show that the softening of the lowest frequency E mode is responsible for the temperature dependence of the dielectric constant, indicating that the ferroelectric transition in BiFeO3 is soft-mode driven.
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