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Register a new userU 5$f$ crystal-field ground state of UO$_2$ probed by directional dichroism in nonresonant inelastic x-ray scattering
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Gerrit van der Laan
Publication date
2018
fields
Physics
and research's language is
English
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Nonresonant inelastic x-ray scattering (NIXS) has been performed on single crystals of UO$_2$ to study the direction dependence of higher-order-multipole scattering from the uranium $O_{4,5}$ edges (90--110 eV). By comparing the experimental results with theoretical calculations the symmetry of the ground state is confirmed directly as the crystal-field (CF) $Gamma_5$ triplet state within the $J$ = 4 manifold. The results also demonstrate that the directional dichroism of the NIXS spectra is sensitive to the CF strength and establish NIXS as a tool for probing CF interactions quantitatively.
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Recent experiments by Larson et al. demonstrate the feasibility of measuring local $dd$ excitations using nonresonant inelastic X-ray scattering (IXS). We establish a general framework for the interpretation where the $dd$ transitions created in the scattering process are expressed in effective one-particle operators that follow a simple selection rule. The different operators can be selectively probed by employing their different dependence on the direction and magnitude of the transferred momentum. We use the operators to explain the presence of nodal directions and the nonresonant IXS in specific directions and planes. We demonstrate how nonresonant IXS can be used to extract valuable ground state information for orbiton excitations in manganite.
TmGa$_{3}$ (AuCu$_3$ structure) undergoes two phase transitions, an antiferroquadrupolar transition at $sim$ 4.29 K and long-range antiferromagnetic ordering at $sim$ 4.26 K. Due to the close vicinity of the two phase transitions, TmGa$_3$ offers an interesting system to study the interplay of charge and magnetic degrees of freedom. In order to understand this interplay we have performed inelastic neutron scattering experiments on TmGa$_{3}$ in the paramagnetic regime ($T >$ 5 K) to redetermine the crystal electric field level scheme. By fitting our spectra at various temperatures we obtain a new crystal field level scheme with Lea, Leask and Wolf parameters of $x_{rm LLW}$ = -0.44(2) and $W$ = -0.222(2) K. The total crystal field splitting at 5K amounts to $sim$ 2.3 meV, about an order of magnitude less than found previously, but in good agreement with the splitting extrapolated from the related ErGa$_3$ system. Our analysis yields a $Gamma_{2}$ singlet as the crystal field ground state followed closely by a (nonmagnetic) $Gamma_{1}$ singlet at 0.009 meV. The next excited states are a $Gamma_{5}^{(2)}$ triplet at $sim$0.5 meV, which is almost degenerate to a $Gamma_{4}$ doublet. This level scheme is adverse to previous findings. Subsequent analysis of the magnetisation along several crystallographic directions and the temperature dependant susceptibility as well as of the magnetic contribution to the specific heat are consistent with our new crystal field parameters. Implications for the antiferroquadrupolar and the antiferromagnetic transition are discussed.
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 investigated the ground state symmetry of the cubic hidden order compound CeB$_6$ by means of core level non-resonant inelastic x-ray scattering (NIXS). The information is obtained from the directional dependence of the scattering function that arises from higher than dipole transitions. Our new method confirms that the ground state is well described using a localized crystal-field model assuming a $Gamma_8$ quartet ground state.
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.
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