We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below TN = 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90• Ir-O-Ir bonds required for dominant Kitaev exchange. [6,7], in which edge-sharing IrO 6 octahedra form a honeycomb lattice [see Fig. 1b)], have been predicted to display novel magnetic states for composite spin-orbital moments coupled via frustrated exchanges. The exchange between neighboring Ir moments (called S i,j , S=1/2) is proposed to be [2]where J K > 0 is an Ising ferromagnetic (FM) term arising from superexchange via the Ir-O-Ir bond, and J 1 > 0 is the antiferromagnetic (AFM) Heisenberg exchange via direct Ir-Ir 5d overlap. Due to the strong spin-orbital admixture the Kitaev term J K couples only the components in the direction γ, normal to the plane of the Ir-O-Ir bond [8,9]. Because of the orthogonal geometry, different spin components along the cubic axes (γ = x, y, z) of the IrO 6 octahedron are coupled for the three bonds emerging out of each site in the honeycomb lattice. This leads to the strongly-frustrated Kitaev-Heisenberg (KH) model [2], which has conventional Néel order [see Fig. 3a)] for large J 1 , a stripy collinear AFM phase [see Fig. 3c)] for 0.4 α 0.8, where α = J K / (J K + 2J 1 ) (exact ground state at α = 1/2), and a quantum spin liquid with Majorana fermion excitations [10] at large J K (α 0.8). Measurements of the spin excitations are very important to determine the overall energy scale and the relevant magnetic interactions, however because Ir is a strong neutron absorber inelastic neutron scattering (INS) experiments are very challenging. Using an optimized setup we here report the first observation of dispersive spin wave excitations of Ir moments via INS. We show that the dispersion can be quantitatively accounted for by including substantial further-neighbor in-plane exchanges, which in turn stabilize zig-zag order. To inform future ab initio studies of microscopic models of the interactions we combine single-crystal xray diffraction with density functional calculations to determine precisely the oxygen positions, which are key in mediating the exchange and controlling the spin-orbital admixture via crystal field effects. We propose a revised crystal structure with much more symmetric IrO 6 octahedra, but with substantial departures from the ideal 90• Ir-O-Ir bonds required for dominant Kitaev exchange [9], and with frequent structural stacking faults. This differs from the currentlyadopted model, used by several band-structure calculations [14,15], with asymme...
In systems with strong electron-lattice coupling, such as manganites, orbital degeneracy is lifted, causing a null expectation value of the orbital magnetic moment. magnetic structure is thus determined by spin-spin superexchange. In titanates, however, with much smaller Jahn-Teller distortions, orbital degeneracy might allow non-zero values of the orbital magnetic moment, and novel forms of ferromagnetic superexchange interaction unique to t 2g electron systems have been theoretically predicted, although their experimental observation has remained elusive. In this paper, we report a new kind of Ti 3 + ferromagnetism at Lamno 3 /srTio 3 epitaxial interfaces. It results from charge transfer to the empty conduction band of the titanate and has spin and orbital contributions evidencing the role of orbital degeneracy. The possibility of tuning magnetic alignment (ferromagnetic or antiferromagnetic) of Ti and mn moments by structural parameters is demonstrated. This result will provide important clues for understanding the effects of orbital degeneracy in superexchange coupling.
We have carried out neutron diffraction, muon spin relaxation ͑SR͒, and inelastic neutron scattering ͑INS͒ investigations on a polycrystalline sample of CeOs 2 Al 10 to investigate the nature of the phase transition observed near 29 K in the resistivity and heat capacity. Our SR data clearly reveal coherent frequency oscillations below 28 K, indicating the presence of an internal field at the muon site, which confirms the long-range magnetic ordering of the Ce moment below 28 K. Upon cooling the sample below 15 K, unusual behavior of the temperature-dependent SR frequencies may indicate either a change in the muon site, consistent with the observation of superstructure reflections in electron diffraction, or a change in the ordered magnetic structure. Neutron diffraction data do not reveal any clear sign of either magnetic Bragg peaks or superlattice reflections. Furthermore, INS measurements clearly reveal the presence of a sharp inelastic excitation near 11 meV between 5 and 26 K, due to opening of a gap in the spin-excitation spectrum, which transforms into a broad response at and above 30 K. The magnitude of the spin gap ͑11 meV͒ as derived from the INS peak position agrees very well with the gap value as estimated from the bulk properties.
We have investigated the noncentrosymmetric tetragonal heavy-fermion antiferromagnetic compound CeCuAl3 (T(N)=2.5 K) using inelastic neutron scattering (INS). Our INS results unequivocally reveal the presence of three magnetic excitations centered at 1.3, 9.8, and 20.5 meV. These spectral features cannot be explained within the framework of crystal-electric-field models and recourse to Kramers' theorem for a 4f(1) Ce(3+) ion. To overcome these interpretational difficulties, we have generalized the vibron model of Thalmeier and Fulde for cubic CeAl(2) to tetragonal point-group symmetry with the theoretically calculated vibron form-factor. This extension provides a satisfactory explanation for the position and intensity of the three observed magnetic excitations in CeCuAl3, as well as their dependence on momentum transfer and temperature. On the basis of our analysis, we attribute the observed series of magnetic excitations to the existence of a vibron quasibound state.
We have carried out muon spin relaxation (SR), neutron diffraction and inelastic neutron scattering (INS) investigations on polycrystalline samples of Ce(Ru 1-x Fe x ) 2 Al 10 (x=0, 0.3, 0.5, 0.8 and 1) to investigate the nature of the ground state (magnetic ordered versus paramagnetic) and the origin of the spin gap formation as evident from the bulk measurements in the end members. Our zero-field SR spectra clearly reveal coherent two-frequency oscillations at low temperature in x=0, 0.3 and 0.5 samples, which confirms the long-range magnetic ordering of the Ce-moment with T N =27, 26 and 21 K respectively. On the other hand the SR spectra of x=0.8 and x=1 down to 1.4 K and 0.045 K, respectively exhibit a temperature independent KuboToyabe term confirming a paramagnetic ground state. The long-range magnetic ordering in x=0.5 below 21 K has been confirmed through the neutron diffraction study. INS measurements of x=0 2 clearly reveal the presence of a sharp inelastic excitation near 8 meV between 5 K and 26 K, due to an opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. Interestingly, at 4.5 K the spin gap excitation broadens in x=0.3 and exhibits two clear peaks at 8.4(3) and 12.0(5) meV in x=0.5. In the x=0.8 sample, which remains paramagnetic down to 1.2 K, there is a clear signature of a spin gap of 10-12 meV at 7 K, with a strong Q-dependent intensity. Evidence of a spin gap of 12.5(5) meV has also been found in x=1.The observation of a spin gap in the paramagnetic samples (x=0.8 and 1) is an interesting finding in this study and it challenges our understanding of the origin of the semiconducting gap in CeT 2 Al 10 (T=Ru and Os) compounds in terms of hybridization gap opening only a small part of the Fermi surface, gapped spin waves, or a spin-dimer gap.
The present work aims at evidencing the "kosmotrope" nature of trehalose through the analysis of inelastic neutron scattering measurements on trehalose and sucrose water solutions at different temperatures. Neutron spectra were collected by using the spectrometer MARI at the ISIS pulsed neutron source of the Rutherford Appleton Laboratory (Chilton, UK). To study the structural modifications induced on the tetrahedral hydrogen-bond network of water by homologous disaccharides, as a first step, the vibrational properties of pure water at different temperatures have been investigated. In particular, the temperature behavior of the intramolecular OH stretching mode has been analyzed. Successively, the vibrational properties for pure water have been compared with those of the sugar water solutions focusing the attention on the tetrahedral network-forming tendency. Finally, the obtained findings have been compared with previous Raman scattering evidences, and the results interpreted in the frame of recent molecular dynamics simulation works.
A favored interpretation of the gamma <--> alpha phase transition in cerium postulates the transformation of the localized 4f state in gamma-Ce to a weakly correlated itinerant 4f band in alpha-Ce. However, results of high-energy neutron inelastic scattering measurements, presented here, show clearly that the magnetic susceptibility response from alpha-Ce follows the Ce3+ form factor despite the large, 30-fold, increase in its spectral width relative to that in gamma-Ce. This observation provides, for the first time, indisputable evidence for the localized character of the 4f state in the alpha phase. The present findings appear consistent with recent calculations combining dynamical mean-field theory with the local density approximation that indicate a strongly correlated 4f state in alpha-Ce. The localized 4f state is also fundamental to the Kondo volume collapse theories for the gamma <--> alpha phase transition in cerium.
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