Using powder neutron diffraction we have discovered an unusual magnetic order-order transition in the Ising spin chain compound Ca3Co2O6. On lowering the temperature an antiferromagnetic phase with propagation vector k=(0.5,-0.5,1) emerges from a hig
her temperature spin density wave structure with k=(0, 0, 1.01). This transition occurs over an unprecedented time-scale of several hours and is never complete.
We have investigated the spin fluctuations in the langasite compound Ba3NbFe3Si2O14 in both the ordered state and as a function of temperature. The low temperature magnetic structure is defined by a spiral phase characterized by magnetic Bragg peaks
at q=(0,0,tau ~ 1/7) onset at TN=27 K as previously reported by Marty et al. The nature of the fluctuations and temperature dependence of the order parameter is consistent with a classical second order phase transition for a two dimensional triangular antiferromagnet. We will show that the physical properties and energy scales including the ordering wavevector, Curie-Weiss temperature, and the spin-waves can be explained through the use of only symmetric exchange constants without the need for the Dzyaloshinskii-Moriya interaction. This is accomplished through a set of ``helical exchange pathways along the c direction imposed by the chiral crystal structure and naturally explains the magnetic diffuse scattering which displays a strong vector chirality up to high temperatures well above the ordering temperature. This illustrates a strong coupling between magnetic and crystalline chirality in this compound.
The magnetic properties of the high temperature alpha form of the CaCr2O4 compound have been investigated for the first time by magnetic susceptibility, specific heat and powder neutron diffraction. The system undergoes a unique magnetic phase transi
tion at 43K to a long range order incommensurate helical phase with magnetic propagation vector k=(0,0.3317(2),0). The magnetic model proposed from neutron diffraction data shows that the plane of rotation of the spins is perpendicular to the wave-vector, and that the magnetic modulation is consistent with two modes belonging to distinct irreducible representations of the group. The magnetic point group 2221 is not compatible with ferroelectricity unlike the CuCrO2 delafossite [Kimura et al., Phys. Rev. B, 78 140401 (2008)] but predicts the existence of quadratic magnetoelectric effects, discussed based on a Landau analysis.
The S=2 anisotropic triangular lattice alpha-NaMnO2 is studied by neutron inelastic scattering. Antiferromagnetic order occurs at T ~ 45 K with opening of a spin gap. The spectral weight of the magnetic dynamics above the gap (Delta ~ 7.5 meV) has be
en analysed by the single-mode approximation. Excellent agreement with the experiment is achieved when a dominant exchange interaction (|J|/k_B ~ 73 K), along the monoclinic b-axis and a sizeable easy-axis magnetic anisotropy (|D|/k_B ~ 3 K) are considered. Despite earlier suggestions for two-dimensional spin interactions, the dynamics illustrate strongly coupled antiferromagnetic S=2 chains and cancellation of the interchain exchange due to the lattice topology. alpha-NaMnO2 therefore represents a model system where the geometric frustration is resolved through the lowering of the dimensionality of the spin interactions.
We have studied the frustrated system YBaCo4O7 generally described as an alternating stacking of Kagome and triangular layers of magnetic ions on a trigonal lattice, by single crystal neutron diffraction experiments above the Neel ordering transition
. Experimental data reveals pronounced magnetic diffuse scattering, which is successfully modeled by direct Monte-Carlo simulations. Long-range magnetic correlations are found along the c-axis, due to the presence of corner-sharing bipyramids, creating quasi one-dimensional order at finite temperature. In contrast, in the Kagome layers ab-plane, the spin-spin correlation function -displaying a short-range 120 degrees configuration- decays rapidly as typically found in spin-liquids. YBaCo4O7 experimentally realizes a new class of two-dimensional frustrated systems where the strong out-of-plane coupling does not lift the in-plane degeneracy, but instead act as an external field.
The origin of the long-wavelength incommensurate magnetic structure of Ca3Co2O6 is discussed considering possible inter-chains super-superexchange paths. The experimental value of the propagation vector k=(0,0,$Delta$) with $Delta$ $>$ 1 can be repro
duced only if one considers the next nearest super-superexchange interaction. A spin-dimer analysis using the Extended-Huckel Tight-Binding method confirms that, despite longer interatomic Co-Co distances, the latter interaction is indeed much stronger. The stability of the observed structure with respect to certain commensurate states is discussed.
We have determined the magnetic structure of the low-temperature incommensurate phase of multiferroic YMn2O5 using single-crystal neutron diffraction. By employing corepresentation analysis, we have ensured full compliance with both symmetry and phys
ical constraints, so that the electrical polarization must lie along the b axis, as observed. The evolution of the spin components and propagation through the commensurate-incommensurate phase boundary points unambiguously at the exchange-striction mechanism as the primary driving force for ferroelectricity.
The weakly interacting S=1/2 dimers system Sr3Cr2O8 has been investigated by powder neutron diffraction and inelastic neutron scattering. Our data reveal a structural phase transition below room temperature corresponding to an antiferro-orbital order
ing with nearly 90 degrees arrangement of the occupied 3z^2-r^2 d-orbital. This configuration leads to a drastic reduction of the inter-dimer exchange energies with respect to the high temperature orbital-disorder state, as shown by a spin-dimer analysis of the super-superexchange interactions performed using the Extended Huckel Tight Binding method. Inelastic neutron scattering reveals the presence of a quasi non-dispersive magnetic excitation at 5.4 meV, in agreement with the picture of weakly-interacting dimers.
We employ neutron spherical polarimetry to determine the nature and population of the coexisting antiferromagnetic domains in multiferroic YMn2O5. By applying an electric field, we prove that reversing the electrical polarization results in the popul
ation inversion of two types of in-plane domains, related to each other by inversion. Our results are completely consistent with the exchange striction mechanism of ferroelectricity, and support a unified model where cycloidal ordering is induced by coupling to the main magnetic order parameter.
