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Register a new userPolarization dependence of x-ray absorption spectra in Na_xCoO_2
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In order to shed light on the electronic structure of Na_xCoO_2, and motivated by recent Co L-edge X-ray absorption spectra (XAS) experiments with polarized light, we calculate the electronic spectrum of a CoO_6 cluster including all interactions between 3d orbitals. We obtain the ground state for two electronic occupations in the cluster that correspond nominally to all O in the O^{-2} oxidation state, and Co^{+3} or Co^{+4}. Then, all excited states obtained by promotion of a Co 2p electron to a 3d electron, and the corresponding matrix elements are calculated. A fit of the observed experimental spectra is good and points out a large Co-O covalency and cubic crystal field effects, that result in low spin Co 3d configurations. Our results indicate that the effective hopping between different Co atoms plays a major role in determining the symmetry of the ground state in the lattice. Remaining quantitative discrepancies with the XAS experiments are expected to come from composition effects of itineracy in the ground and excited states.
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Measurements of polarization and temperature dependent soft x-ray absorption have been performed on Na_xCoO_2 single crystals with x=0.4 and x=0.6. They show a deviation of the local trigonal symmetry of the CoO_6 octahedra, which is temperature independent in a temperature range between 25 K and 372 K. This deviation was found to be different for Co^{3+} and Co^{4+} sites. With the help of a cluster calculation we are able to interpret the Co L_{23}-edge absorption spectrum and find a doping dependent energy splitting between the t_{2g} and the e_g levels (10Dq) in Na_xCoO_2.
The polarization of x-rays plays an outstanding role in experimental techniques such as non-resonant magnetic x-ray scattering and resonant x-ray scattering of magnetic and multipolar order. Different instrumental methods applied to synchrotron light can transform its natural polarization into an arbitrary polarization state. Several synchrotron applications, in particular in the field of magnetic and resonant scattering rely on the improvement in the signal/noise ratio or the deeper insight into the ordered state and the scattering process made possible through these polarization techniques. Here, we present the mathematical framework for the description of fully and partially polarized x-rays, with some applications such as linear x-ray polarization analysis for the determination of the scattered beams polarization, and the Ge K-edge resonant scattering.
We demonstrate a new method of x-ray absorption spectroscopy (XAS) that is bulk sensitive, like traditional fluorescence yield measurements, but is not affected by self-absorption or saturation effects. This measure of XAS is achieved by scanning the incident photon energy through an absorption edge and using an energy sensitive photon detector to measure the partial fluorescence yield (PFY). The x-ray emission from any element or core-hole excitation that is not resonant with the absorption edge under investigation is selected from the PFY. It is found that the inverse of this PFY spectrum, which we term inverse partial fluorescence yield (IPFY), is linearly proportional to the x-ray absorption cross-section without any corrections due to saturation or self-absorption effects. We demonstrate this technique on the Cu L and Nd M absorption edges of the high-Tc cuprate LNSCO by measuring the O K PFY and comparing the total electron yield, total fluorescence yield and IPFY spectra.
Studying the local moment and 5$f$-electron occupations sheds insight into the electronic behavior in actinide materials. X-ray absorption spectroscopy (XAS) has been a powerful tool to reveal the valence electronic structure when assisted with theoretical calculations. However, the analysis currently taken in the community on the branching ratio of the XAS spectra generally does not account for the hybridization effects between local $f$-orbitals and conduction states. In this paper, we discuss an approach which employs the DFT+Gutzwiller rotationally-invariant slave boson (DFT+GRISB) method to obtain a local Hamiltonian for the single-impurity Anderson model (SIAM), and calculates the XAS spectra by the exact diagonalization (ED) method. A customized numerical routine was implemented for the ED XAS part of the calculation. By applying this technique to the recently discovered 5$f$-electron topological Kondo insulator PuB$_4$, we determined the signature of 5$f$-electronic correlation effects in the theoretical X-ray spectra. We found that the Pu 5$f$-6$d$ hybridization effect provides an extra channel to mix the $j=5/2$ and $7/2$ orbitals in the 5$f$ valence. As a consequence, the resulting electron occupation number and spin-orbit coupling strength deviate from the intermediate coupling regime.
An alternative measure of x-ray absorption spectroscopy (XAS) called inverse partial fluorescence yield (IPFY) has recently been developed that is both bulk sensitive and free of saturation effects. Here we show that the angle dependence of IPFY can provide a measure directly proportional to the total x-ray absorption coefficient, $mu(E)$. In contrast, fluorescence yield (FY) and electron yield (EY) spectra are offset and/or distorted from $mu(E)$ by an unknown and difficult to measure amount. Moreover, our measurement can determine $mu(E)$ in absolute units with no free parameters by scaling to $mu(E)$ at the non-resonant emission energy. We demonstrate this technique with measurements on NiO and NdGaO$_3$. Determining $mu(E)$ across edge-steps enables the use of XAS as a non-destructive measure of material composition. In NdGaO$_3$, we also demonstrate the utility of IPFY for insulating samples, where neither EY or FY provide reliable spectra due to sample charging and self-absorption effects, respectively.
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