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Register a new user5d-5f Electric-multipole Transitions in Uranium Dioxide Probed by Non-resonant Inelastic X-ray Scattering
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Non-resonant inelastic x ray scattering (NIXS) experiments have been performed to probe the 5d-5f electronic transitions at the uranium O(4,5) absorption edges in uranium dioxide. For small values of the scattering vector q, the spectra are dominated by dipole-allowed transitions encapsulated within the giant resonance, whereas for higher values of q the multipolar transitions of rank 3 and 5 give rise to strong and well-defined multiplet structure in the pre-edge region. The origin of the observed non-dipole multiplet structures is explained on the basis of many-electron atomic spectral calculations. The results obtained demonstrate the high potential of NIXS as a bulk-sensitive technique for the characterization of the electronic properties of actinide materials.
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Strongly correlated materials are characterized by the presence of electron-electron interactions in their electronic structure. They often have remarkable properties and transitions between competing phases of very different electronic and magnetic order. This thesis focuses on strongly correlated $f$-electron compounds containing Ce, Sm, and U. These materials exhibit a so-called heavy-fermion or Kondo-lattice behavior. They can become insulating due to hybridization effects (Kondo-insulator) or develop multipolar (hidden) order. Kondo insulators have recently been discussed in the context of strongly correlated topological insulators. This new aspect caused an enormous activity in the field of Kondo insulators, theoretically as well as experimentally. Multipolar order as well as the formation of a Kondo insulating state strongly depend on the symmetry of the $f$ states involved. Also the character of the surface states in a topological insulator is determined by the properties of the bulk states. Therefore the scope of this thesis has been to unveil the underlying symmetries of the bulk $f$ states. Here the compounds CeB$_6$, UO$_2$, and URu$_2$Si$_2$, which exhibit multipolar order, as well as the Kondo insulators (semimetals) SmB$_6$ and CeRu$_4$Sn$_6$ have been studied.
We report a high-resolution resonant inelastic x-ray scattering study of La2CuO4. A number of spectral features are identified that were not clearly visible in earlier lower-resolution data. The momentum dependence of the spectral weight and the dispersion of the lowest energy excitation across the insulating gap have been measured in detail. The temperature dependence of the spectral features was also examined. The observed charge transfer edge shift, along with the low dispersion of the first charge transfer excitation are attributed to the lattice motion being coupled to the electronic system. In addition, we observe a dispersionless feature at 1.8 eV, which is associated with a d-d crystal field excitation.
Multiferroic TbMnO3 is investigated using x-ray diffraction in high magnetic fields. Measurements on first and second harmonic structural reflections due to modulations induced by the Mn and Tb magnetic order are presented as function of temperature and field oriented along the a and b-directions of the crystal. The relation to changes in ordering of the rare earth moments in applied field is discussed. Observations below T_N(Tb) without and with applied magnetic field point to a strong interaction of the rare earth order, the Mn moments and the lattice. Also, the incommensurate to commensurate transition of the wave vector at the critical fields is discussed with respect to the Tb and Mn magnetic order and a phase diagram on basis of these observations for magnetic fields H||a and H||b is presented. The observations point to a complicated and delicate magneto-elastic interaction as function of temperature and field.
The parent compounds of iron-based superconductors are magnetically-ordered bad metals, with superconductivity appearing near a putative magnetic quantum critical point. The presence of both Hubbard repulsion and Hunds coupling leads to rich physics in these multiorbital systems, and motivated descriptions of magnetism in terms of itinerant electrons or localized spins. The NaFe$_{1-x}$Cu$_x$As series consists of magnetically-ordered bad metal ($x=0$), superconducting ($xapprox0.02$) and magnetically-ordered semiconducing/insulating ($xapprox0.5$) phases, providing a platform to investigate the connection between superconductivity, magnetism and electronic correlations. Here we use X-ray absorption spectroscopy and resonant inelastic X-ray scattering to study the valence state of Fe and spin dynamics in two NaFe$_{1-x}$Cu$_x$As compounds ($x=0$ and 0.47). We find that magnetism in both compounds arises from Fe$^{2+}$ atoms, and exhibits underdamped dispersive spin waves in their respective ordered states. The dispersion of spin excitations in NaFe$_{0.53}$Cu$_{0.47}$As is consistent with being quasi-one-dimensional. Compared to NaFeAs, the band top of spin waves in NaFe$_{0.53}$Cu$_{0.47}$As is slightly softened with significantly more spectral weight of the spin excitations. Our results indicate the spin dynamics in NaFe$_{0.53}$Cu$_{0.47}$As arise from localized magnetic moments and suggest the iron-based superconductors are proximate to a correlated insulating state with localized iron moments.
Resonant inelastic x-ray scattering (RIXS) at the oxygen $K$-edge has recently accessed multi-spinon excitations in the one-dimensional antiferromagnet (1D-AFM) sco, where four-spinon excitations are resolved separately from the two-spinon continuum. This technique, therefore, provides new opportunities to study fractionalized quasiparticle excitations in doped 1D-AFMs. To this end, we carried out exact diagonalization studies of the doped $t$-$J$ model and provided predictions for oxygen $K$-edge RIXS experiments on doped 1D-AFMs. We show that the RIXS spectra are rich, containing distinct two- and four-spinon excitations, dispersive (anti)holon excitations, and combinations thereof. Our results highlight how RIXS complements inelastic neutron scattering experiments by accessing additional charge and spin components of fractionalized quasiparticles.
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