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On the magnetoelastic and magnetoelectric couplings across the antiferromagnetic transition in multiferroic BiFeO3

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 Added by Pascal Ruello
 Publication date 2018
  fields Physics
and research's language is English




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Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice change at T_N as a result of magnetostriction combined with electrostrictive and magnetoelectric couplings which renormalize the elastic constants of the high-temperature reference phase when the critical T_N temperature is reached.



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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.
Complex experimental and theoretical study of the magnetic, magnetoelectric, and magnetoelastic properties of neodymium iron borate NdFe3(BO3)4 along various crystallographic directions have been carried out in strong pulsed magnetic fields up to 230 kOe in a temperature range of 4.2-50 K. It has been found that neodymium iron borate, as well as gadolinium iron borate, is a multiferroic. It has much larger (above 3 10^(-4) C/m^2) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (~50 kOe) has been determined for the first time from experimental data. The theoretical analysis based on the magnetic symmetry and quantum properties of the Nd ion in the crystal provides an explanation of an unusual behavior of the magnetoelectric and magnetoelastic properties of neodymium iron borate in strong magnetic fields and correlation observed between them.
Multiferroic BiFeO3 ceramics have been doped with Ca. The smaller ionic size of Ca compared with Bi means that doping acts as a proxy for hydrostatic pressure, at a rate of 1%Ca=0.3GPa. It is also found that the magnetic Neel temperature (TNeel) increases as Ca concentration increases, at a rate of 0.66K per 1%Ca (molar). Based on the effect of chemical pressure on TNeel, we argue that applying hydrostatic pressure to pure BiFeO3 can be expected to increase its magnetic transition temperature at a rate around ~2.2K/GPa. The results also suggest that pressure (chemical or hydrostatic) could be used to bring the ferroelectric critical temperature, Tc, and the magnetic TNeel closer together, thereby enhancing magnetoelectric coupling, provided that electrical conductivity can be kept sufficiently low.
We report X-ray structural studies of the metal-insulator phase transition in bismuth ferrite, BiFeO3, both as a function of temperature and of pressure (931 oC at atmospheric pressure and ca. 45 GPa at ambient temperature). Based on the experimental results, we argue that the metallic gamma-phase is not rhombohedral but is instead the same cubic Pm3m structure whether obtained via high temperature or high pressure, that the MI transition is second order or very nearly so, that this is a band-type transition due to semi-metal band overlap in the cubic phase and not a Mott transition, and that it is primarily structural and not an S=5/2 to S=1/2 high-spin/low-spin electronic transition. Our data are compatible with the orthorhombic Pbnm structure for the beta-phase determined definitively by the neutron scattering study of Arnold et al .[Phys. Rev. Lett. 2009]; the details of this beta-phase had also been controversial, with a remarkable collection of five crystal classes (cubic, tetragonal, orthorhombic, monoclinic, and rhombohedral!) all claimed in recent publications.
We report a temperature-dependent Raman and neutron scattering investigation of the multiferroic material bismuth ferrite BiFeO3 (BFO).
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