Symmetry, incommensurate magnetism and ferroelectricity: the case of the rare-earth manganites RMnO3

The complete irreducible co-representations of the paramagnetic space group provide a simple and direct path to explore the symmetry restrictions of magnetically driven ferroelectricity. The method consists of a straightforward generalization of the method commonly used in the case of displacive modulated systems and allows us to determine, in a simple manner, the full magnetic symmetry of a given phase originated from a given magnetic order parameter. The potential ferroic and magneto-electric properties of that phase can then be established and the exact Landau free energy expansions can be derived from general symmetry considerations. In this work, this method is applied to the case of the orthorhombic rare-earth manganites RMnO3. This example will allow us to stress some specific points, such as the differences between commensurate or incommensurate magnetic phases regarding the ferroic and magnetoelectric properties, the possible stabilization of ferroelectricity by a single irreducible order parameter or the possible onset of a polarization oriented parallel to the magnetic modulation. The specific example of TbMnO3 will be considered in more detail, in order to characterize the role played by the magneto-electric effect in the mechanism for the polarization rotation induced by an external magnetic field.Comment: Conference: Aperiodic`0

Magnetic frustration in the spinel compounds Ge Co_2 O_4 and Ge Ni_2 O_4

In both spinel compounds GeCo$_2$O$_4$ and GeNi$_2$O$_4$ which order antiferromagnetically (at $T_N = 23.5 K$ and $T_{N_1} = 12.13 K$, $T_{N_2} = 11.46 K$) with different Curie Weiss temperatures ($T_{CW}$=80.5 K and -15 K), the usual magnetic frustration criterion $f=|T_{CW}|/T_N>>1$ is not fulfilled. Using neutron powder diffraction and magnetization measurements up to 55 T, both compounds are found with a close magnetic ground state at low temperature and a similar magnetic behavior (but with a different energy scale), even though spin anisotropy and first neighbor exchange interactions are quite different. This magnetic behavior can be understood when considering the main four magnetic exchange interactions. Frustration mechanisms are then enlightened.Comment: submitted to Phys.Rev.B (2006

Coupling of phonons and electromagnons in GdMnO_3

The infrared and Terahertz properties of GdMnO_3 have been investigated as function of temperature and magnetic field, with special emphasis on the phase boundary between the incommensurate and the canted antiferromagnetic structures. The heterogeneous incommensurate phase reveals strong magnetodielectric effects, characterized by significant magnetoelectric contributions to the static dielectric permittivity and by the existence of electrically excited magnons (electromagnons). In the commensurate canted antiferromagnetic phase the magnetoelectric contributions to the dielectric constant and electromagnons are suppressed. The corresponding spectral weight is transferred to the lowest lattice vibration demonstrating the strong coupling of phonons with electromagnons.Comment: 5 pages, 4 figure

Non collinear magnetism and single ion anisotropy in multiferroic perovskites

The link between the crystal distortions of the perovskite structure and the magnetic exchange interaction, the single-ion anisotropy (SIA) and the Dzyaloshinsky-Moriya (DM) interaction are investigated by means of density-functional calculations. Using BiFeO$_3$ and LaFeO$_3$ as model systems, we quantify the relationship between the oxygen octahedra rotations, the ferroelectricity and the weak ferromagnetism (wFM). We recover the fact that the wFM is due to the DM interaction induced by the oxygen octahedra rotations. We find a simple relationship between the wFM, the oxygen rotation amplitude and the ratio between the DM vector and the exchange parameter such as the wFM increases with the oxygen octahedra rotation when the SIA does not compete with the DM forces induced on the spins. Unexpectedly, we also find that, in spite of the $d^5$ electronic configuration of Fe$^{3+}$, the SIA is very large in some structures and is surprisingly strongly sensitive to the chemistry of the $A$-site cation of the $A$BO$_3$ perovskite. In the ground $R3c$ state phase we show that the SIA shape induced by the ferroelectricity and the oxygen octahedra rotations are in competition such as it is possible to tune the wFM "on" and "off" through the relative size of the two types of distortion

Coupling of frustrated Ising spins to magnetic cycloid in multiferroic TbMnO3

We report on diffraction measurements on multiferroic TbMnO3 which demonstrate that the Tb- and Mn-magnetic orders are coupled below the ferroelectric transition TFE = 28 K. For T < TFE the magnetic propagation vectors (tau) for Tb and Mn are locked so that tauTb = tauMn, while below TNTb = 7 K we find that tauTb and tauMn lock-in to rational values of 3/7 b* and 2/7 b*, respectively, and obey the relation 3tauTb - tauMn = 1. We explain this novel matching of wave vectors within the frustrated ANNNI model coupled to a periodic external field produced by the Mn-spin order. The tauTb = tauMn behavior is recovered when Tb magnetization is small, while the tauTb = 3/7 regime is stabilized at low temperatures by a peculiar arrangement of domain walls in the ordered state of Ising-like Tb spins.Comment: 5 pages, 3 figure

Ga substitution as an effective variation of Mn-Tb coupling in multiferroic TbMnO3

Ga for Mn substitution in multiferroic TbMnO$_{3}$ has been performed in order to study the influence of Mn-magnetic ordering on the Tb-magnetic sublattice. Complete characterization of TbMn$_{1-x}$Ga$_x$O$_{3}$ ($x$ = 0, 0.04, 0.1) samples, including magnetization, impedance spectroscopy, and x-ray resonant scattering and neutron diffraction on powder and single crystals has been carried out. We found that keeping the same crystal structure for all compositions, Ga for Mn substitution leads to the linear decrease of $T_{\rm N}^{\rm Mn}$ and $\tau^{\rm Mn}$, reflecting the reduction of the exchange interactions strength $J_{\rm Mn-Mn}$ and the change of the Mn-O-Mn bond angles. At the same time, a strong suppression of both the induced and the separate Tb-magnetic ordering has been observed. This behavior unambiguously prove that the exchange fields $J_{\rm Mn-Tb}$ have a strong influence on the Tb-magnetic ordering in the full temperature range below $T_{\rm N}^{\rm Mn}$ and actually stabilize the Tb-magnetic ground state.Comment: 9 pages, 8 figure

Magnetization Reversal by Electric-Field Decoupling of Magnetic and Ferroelectric Domains Walls in Multiferroic-Based Heterostructures

We demonstrate that the magnetization of a ferromagnet in contact with an antiferromagnetic multiferroic (LuMnO3) can be speedily reversed by electric field pulsing, and the sign of the magnetic exchange bias can switch and recover isothermally. As LuMnO3 is not ferroelastic, our data conclusively show that this switching is not mediated by strain effects but is a unique electric-field driven decoupling of the ferroelectric and ferromagnetic domains walls. Their distinct dynamics are essential for the observed magnetic switching

Spin fluctuations in the stacked-triangular antiferromagnet YMnO3

The spectrum of spin fluctuations in the stacked-triangular antiferromagnet YMnO3 was studied above the Neel temperature using both unpolarized and polarized inelastic neutron scattering. We find an in-plane and an out-of-plane excitation. The in-plane mode has two components just above TN, a resolution-limited central peak and a Debye-like contribution. The quasi-elastic fluctuations have a line-width that increases with q like Dq^z and the dynamical exponent z=2.3. The out-of-plane fluctuations have a gap at the magnetic zone center and do not show any appreciable q-dependence at small wave-vectors.Comment: JETP LETTERS, in pres

Crystal structure and high-field magnetism of La2CuO4

Neutron diffraction was used to determine the crystal structure and magnetic ordering pattern of a La2CuO4 single crystal, with and without applied magnetic field. A previously unreported, subtle monoclinic distortion of the crystal structure away from the orthorhombic space group Bmab was detected. The distortion is also present in lightly Sr-doped crystals. A refinement of the crystal structure shows that the deviation from orthorhombic symmetry is predominantly determined by displacements of the apical oxygen atoms. An in-plane magnetic field is observed to drive a continuous reorientation of the copper spins from the orthorhombic b-axis to the c-axis, directly confirming predictions based on prior magnetoresistance and Raman scattering experiments. A spin-flop transition induced by a c-axis oriented field previously reported for non-stoichiometric La2CuO4 is also observed, but the transition field (11.5 T) is significantly larger than that in the previous work

Magnetic Structure Investigations at the Nuclear Center

The magnetic structure of the compounds UOS, ß-CoSO4, YCO5, and HoCO5 is briefly described. UOS is antiferromagnetic. The Néel temperature is Tn=55°K. The magnetic cell is doubled in the c direction with a ++ - - sequence of U moments along c. The apparent spin is S∼1. The negative interaction corresponds to U-O-U links. In ß-CoSO4 (high-temperature modification, space group Pbnm), Co atoms are in 000, 00½, ½½½, ½½0. Here three different antiferromagnetic spin modes, mutually perpendicular, Ax(+ - - +), Gy(+-+-), and Cz(++ - - ), in the Wollan-Koehler notation, are coupled. Direction cosines are 0.71, 0.50, and 0.50, respectively. The Co moment is about 3,84 µB at 4.2°K. A field-induced spin flip to the configuration Fx, Cy, Gz is predicted. YCO5 is ferromagnetic at room temperature with a moment value of Co practically equal to that of metallic Co and moment direction along c, which is conserved down to 4.2°K. In HoCO5 the moment of Ho is opposite to those of the Co atoms. When cooling from room to liquid helium temperature, the direction of easy magnetization changes from near c to a direction in the basal plane and the Ho moment increases from 4 to about 9 µB. The compensation temperature is 70°K