We have performed Raman scattering investigations on the high energy magnetic excitations in a BiFeO$_3$ single crystal as a function of both temperature and laser excitation energy. A strong feature observed at 1250 cm$^{-1}$ in the Raman spectra ha
s been previously assigned to two phonon overtone. We show here that its unusual frequency shift with the excitation energy and its asymmetric temperature dependent Fano lineshape reveal a strong coupling to magnetic excitations. In the same energy range, we have also identified the two-magnon excitation with a temperature dependence very similar to $alpha$-Fe$_2$O$_3$ hematite.
Bismuth ferrite, BiFeO3, is the only known room-temperature multiferroic material. We demonstrate here, using neutron scattering measurements in high quality single crystals, that the antiferromagnetic and ferroelectric orders are intimately coupled.
Initially in a single ferroelectric state, our crystals have a canted antiferromagnetic structure describing a unique cycloid. Under electrical poling, polarisation re-orientation induces a spin flop. We argue here that the coupling between the two orders may be stronger in the bulk than that observed in thin films where the cycloid is absent.
Micro-Raman spectroscopy has been used to study lattice dynamics associated with the ferroelectric domains of a BiFeO$_3$ single crystal at low temperature. The phonon assignment shows a large frequency splitting between the transverse and longitudin
al components of the A$_1$ phonon mode related to the Bi-O bonds in contrast with thin films where the splitting is negligible. Applying an external electric field induces frequency shifts of the low energy modes related to the Bi-O bonds. These softenings are due to a tensile stress via the piezoelectric effect. We give estimates of the phonon deformation potentials.
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.
Electric polarization loops are measured at room temperature on highly pure BiFeO3 single crystals synthesized by a flux growth method. Because the crystals have a high electrical resistivity, the resulting low leakage currents allow us to measure a
large spontaneous polarization reaching 100 microC.cm^{-2}, a value never reported in the bulk. During electric cycling, the slow degradation of the material leads to an evolution of the hysteresis curves eventually preventing full saturation of the crystals.
