Using a recently developed impurity solver we exemplify how dynamical mean field theory captures band excitations, resonances, edge singularities and excitons in core level x-ray absorption (XAS) and core level photo electron spectroscopy (cPES) on m
etals, correlated metals and Mott insulators. Comparing XAS at different values of the core-valence interaction shows how the quasiparticle peak in the absence of core-valence interactions evolves into a resonance of similar shape, but different origin. Whereas XAS is rather insensitive to the metal insulator transition, cPES can be used, due to nonlocal screening, to measure the amount of local charge fluctuation.
A combined analysis of x-ray absorption and resonant reflectivity data was used to obtain the orbital polarization profiles of superlattices composed of four-unit-cell-thick layers of metallic LaNiO3 and layers of insulating RXO3 (R=La, Gd, Dy and X=
Al, Ga, Sc), grown on substrates that impose either compressive or tensile strain. This superlattice geometry allowed us to partly separate the influence of epitaxial strain from interfacial effects controlled by the chemical composition of the insulating blocking layers. Our quantitative analysis reveal orbital polarizations up to 25%. We further show that strain is the most effective control parameter, whereas the influence of the chemical composition of the blocking layers is comparatively small.
We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on th
in films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.
We study the magnetic susceptibility of mixed-valent La2-xSrxCoO4 single crystals in the doping range of 0.5<= x <= 0.8 for temperatures up to 1000 K. The magnetism below room temperature is described by paramagnetic Co2+ in the high-spin state and b
y Co3+ in the non-magnetic low-spin state. Above room temperature, an increase in susceptibility compared to the behavior expected from Co2+ is seen, which we attribute to a spin-state transition of Co3+. The susceptibility is analyzed by comparison to full-multiplet calculations for the thermal population of the high- and intermediate-spin states of Co3+.
The occupation of d-orbitals controls the magnitude and anisotropy of the inter-atomic electron transfer in transition metal oxides and hence exerts a key influence on their chemical bonding and physical properties. Atomic-scale modulations of the or
bital occupation at surfaces and interfaces are believed to be responsible for massive variations of the magnetic and transport properties, but could thus far not be probed in a quantitative manner. Here we show that it is possible to derive quantitative, spatially resolved orbital polarization profiles from soft x-ray reflectivity data, without resorting to model calculations. We demonstrate that the method is sensitive enough to resolve differences of 3 % in the occupation of Ni e_g orbitals in adjacent atomic layers of a LaNiO3-LaAlO3 superlattice, in good agreement with ab-initio electronic-structure calculations. The possibility to quantitatively correlate theory and experiment on the atomic scale opens up many new perspectives for orbital physics in d-electron materials.
We report on the local electronic structure of Fe impurities in MgO thin films. Using soft x-ray absorption spectroscopy (XAS) we verified that the Fe impurities are all in the 2+ valence state. The fine details in the line shape of the Fe $L_{2,3}$
edges provide direct evidence for the presence of a dynamical Jahn-Teller distortion. We are able to determine the magnitude of the effective $D_{4h}$ crystal field energies. We also observed a strong temperature dependence in the spectra which we can attribute to the thermal population of low-lying excited states that are present due to the spin-orbit coupling in the Fe 3d. Using this Fe$^{2+}$ impurity system as an example, we show that an accurate measurement of the orbital moment in Fe$_3$O$_4$ will provide a direct estimate for the effective local low-symmetry crystal fields on the Fe$^{2+}$ sites, important for the theoretical modeling of the formation of orbital ordering.
A general symmetry analysis of the optical conductivity or scattering tensor is used to rewrite the conductivity tensor as a sum of fundamental spectra multiplied by simple functions depending on the local magnetization direction. Using this formalis
m, we present several numerical examples at the transition metal L23 edge. From these numerical calculations we can conclude that large deviations from the magneto-optical effects in spherical symmetry are found. These findings are in particular important for resonant x-ray diffraction experiments where the polarization dependence and azimuthal dependence of the scattered Bragg intensity is used to determine the local ordered magnetization direction.
We have measured the intricate temperature dependence of the Co L2,3 x-ray absorption spectra (2p-3d excitations) of CoO. To allow for accurate total electron yield measurements, the material has been grown in thin film form on a metallic substrate i
n order to avoid charging problems usually encountered during electron spectroscopic studies on bulk CoO samples. The changes in spectra due to temperature are in good agreement with detailed ligand-field calculations indicating that these changes are mostly due to thermal population of closely lying excited states, originating from degenerate t2g levels lifted by the spin-orbit coupling. Magnetic coupling in the ordered phase, modeled as a mean-field exchange field, mixes in excited states inducing a tetragonal charge density. The spin-orbit coupling induced splitting of the low energy states results in a non-trivial temperature dependence for the magnetic susceptibility.
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.
We compare for Ho metal the x-ray absorption spectrum and the resonant soft x-ray diffraction spectra obtained at the $3d_{5/2} to 4f$ ($M_5$) resonance for the magnetic 1st and 2nd order diffraction peaks $(0,0,tau)$ and $(0,0,2tau)$ with the result
of an atomic multiplet calculation. We find a good agreement between experiment and simulation giving evidence that this kind of simulation is well suited to quantitatively analyze resonant soft x-ray diffraction data from correlated electron systems.
