Lattice dynamics of BaFe2Se3.

This paper presents a study of the lattice dynamics in BaFe2Se3. We combined first-principle calculations, infrared measurements and a thorough symmetry analysis. Our study confirms thatPnmacannot be the space group of BaFe2Se3, even at room temperature. The phonons assignment requiresPmto be the BaFe2Se3space group, not only in the magnetic phase, but also in the paramagnetic phase at room temperature. This is due to a strong coupling between a short-range spin-order along the ladders, and the lattice degrees of freedom associated with the Fe-Fe bond length. This coupling induces a change in the bond-length pattern from an alternated trapezoidal one (as inPnma) to an alternated small/large rectangular one. Out of the two patterns, only the latter is fully compatible with the observed block-type magnetic structure. Finally, we propose a complete symmetry analysis of the BaFe2Se3phase diagram in the 0-600 K range.

Analysis of the magnetic properties of Ce3Pt23Si11: orthorhombic crystal field and mean-field approximation.

We present here a quantitative analysis of the ground state and magnetic properties of Ce3Pt23Si11, based on a crystalline electric field description within the mean-field approximation. In this face-centered cubic compound, the point group symmetry at the Ce site is orthorhombic. One main difficulty in this low symmetry case is that the CEF potential for Ce3+ ions is determined by five independent parameters, while only two magnetic excitations are observed by inelastic neutron scattering. Moreover the anisotropy of the magnetic susceptibility of the Ce ion, that permits an independent determination of the second-order CEF parameters is hidden by the cubic symmetry of the compound. A specific procedure is developed for this purpose that combines genetic algorithms and more conventional optimization methods. A set of CEF parameters is found that best reproduces the different experimental observations in both the paramagnetic and ferromagnetic phases of Ce3Pt23Si11. The analysis accounts for two seemingly contradictory properties: a strong local anisotropy that aligns the moment along a fourfold axis and a rather weak anisotropy of the bulk magnetization with an easy threefold magnetization axis. Ce3Pt23Si11 is shown to be a model system where single site anisotropies compete within a crystal structure of overall high symmetry.

3d-4f coupling and multiferroicity in frustrated Cairo Pentagonal oxide DyMn2O5.

In solid state science, multifunctional materials and especially multiferroics have attracted a great deal of attention, as they open the possibility for next generation spintronic and data storage devices. Interestingly, while many of them host coexisting 3d and 4f elements, the role of the coupling between these two magnetic entities has remained elusive. By means of single crystal neutron diffraction and inelastic neutron scattering experiments we shed light on this issue in the particular case of the multiferroic oxide DyMn2O5. This compound undergoes a first order magnetic transition from a high temperature incommensurate phase to a low temperature commensurate one. Our investigation reveals that although these two phases have very different magnetic structures, the spin excitations are quite similar indicating a fragile low temperature ground state with respect to the high temperature one. Such a rare scenario is argued to be a manifestation of the competition between the exchange interaction and 4f magnetic anisotropy present in the system. It is concluded that the magnetic structure, hence the ferroelectricity, can be finely tuned depending on the anisotropy of the rare earth.

Evidence for room temperature electric polarization in RMn(2)O(5) multiferroics.

It is established that the multiferroics RMn(2)O(5) crystallize in the centrosymmetric Pbam space group and that the magnetically induced electric polarization appearing at low temperature is accompanied by a symmetry breaking. However, both our present x-ray study-performed on compounds with R=Pr,Nd,Gd,Tb, and Dy-and first-principles calculations unambiguously rule out this picture. Based on structural refinements, geometry optimization, and physical arguments, we demonstrate in this Letter that the actual space group is likely to be Pm. This turns out to be of crucial importance for RMn(2)O(5) multiferroics since Pm is not centrosymmetric. Ferroelectricity is thus already present at room temperature, and its enhancement at low temperature is a spin-enhanced process. This result is also supported by direct observation of optical second harmonic generation. This fundamental result calls into question the actual theoretical approaches that describe the magnetoelectric coupling in this multiferroic family.

An ab initio study of magneto-electric coupling of YMnO3.

This paper proposes the direct calculation of the microscopic contributions to the magneto-electric coupling, using ab initio methods. The electrostrictive and the Dzyaloshinskii-Moriya contributions were evaluated individually. For this purpose a specific method was designed, combining density functional theory calculations and embedded fragment, explicitly correlated, quantum chemical calculations. This method allowed us to calculate the evolution of the magnetic couplings as a function of an applied electric field. We found that in YMnO3 the Dzyaloshinskii-Moriya contribution to the magneto-electric effect is three orders of magnitude weaker than the electrostrictive contribution. Strictive effects are thus dominant in the magnetic exchange evolution under an applied electric field, and by extension in the magneto-electric effect. These effects however, remain quite small, and the modifications of the magnetic excitations under an applied electric field will be difficult to observe experimentally. Another important conclusion is that it can be shown that the linear magneto-electric tensor is null due to the inter-layer symmetry operations.