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We report resonant X-ray scattering measurements on the orbitally-degenerate triangular metallic antiferromagnet 2H-AgNiO2 to probe the spontaneous transition to a triple-cell superstructure at temperatures below 365 K. We observe a strong resonant e nhancement of the supercell reflections through the Ni K-edge. The empirically extracted K-edge shift between the crystallographically-distinct Ni sites of 2.5(3) eV is much larger than the value expected from the shift in final states, and implies a core-level shift of ~1 eV, thus providing direct evidence for the onset of spontaneous honeycomb charge order in the triangular Ni layers. We also provide band-structure calculations that explain quantitatively the observed edge shifts in terms of changes in the Ni electronic energy levels due to charge order and hybridization with the surrounding oxygens.
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.
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.
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