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Resonant inelastic x-ray scattering study of charge excitations in La2CuO4

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 Added by Young-June Kim
 Publication date 2002
  fields Physics
and research's language is English




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We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $sim 2.2$ eV at the zone center, and a dispersion of $sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($pi$, $pi$). The second peak shows a smaller dispersion ($sim 0.5$ eV) with a zone-center energy of $sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the presence of the electron-hole continuum.

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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.
We analyze the resonant inelastic x-ray scattering (RIXS) spectra at the Cu and Ni K edges in La2CuO4 and La2NiO4, respectively. We make use of the Keldysh-Green-function formalism, in which the RIXS intensity is described by a product of incident-photon-dependent factor and density-density correlation function in the 3d states. The former factor is calculated using the $4p$ density of states given by an ab initio band structure calculation and the latter using the wavefunctions given by a Hartree-Fock calculation of a multi-orbital tight-binding model. The initial state is described within the Hartree-Fock approximation and the electron correlations on charge excitations are treated within the random phase approximation. The calculated RIXS spectra well reproduce several characteristic features in the experiments. Although several groups have interpreted the RIXS peaks as bound excitons, our calculation indicates that they should be interpreted as band-to-band excitations augmented by electron correlations. The difference in RIXS spectra between La2CuO4 and La2NiO4 is explained from this point of view.
Resonant inelastic X-ray scattering (RIXS) is a powerful probe of elementary excitations in solids. It is now widely applied to study magnetic excitations. However, its complex cross-section means that RIXS has been more difficult to interpret than inelastic neutron scattering (INS). Here we report high-resolution RIXS measurements of magnetic excitations of La2CuO4, the antiferromagnetic parent of one system of high-temperature superconductors. At high energies (~2 eV), the RIXS spectra show angular-dependent dd orbital excitations which are found to be in good agreement with single-site multiplet calculations. At lower energies (<0.3 eV), we show that the wavevector-dependent RIXS intensities are proportional to the product of the single-ion spin-flip cross section and the dynamical susceptibility of the spin-wave excitations. When the spin-flip crosssection is dividing out, the RIXS magnon intensities show a remarkable resemblance to INS data. Our results show that RIXS is a quantitative probe the dynamical spin susceptibility in cuprate and therefore should be used for quantitative investigation of other correlated electron materials.
151 - T. Nomura , Y. Harada , H. Niwa 2016
Low-energy electron excitation spectra were measured on a single crystal of a typical iron-based superconductor PrFeAsO$_{0.7}$ using resonant inelastic X-ray scattering (RIXS) at the Fe-$L_3$ edge. Characteristic RIXS features are clearly observed around 0.5, 1-1.5 and 2-3 eV energy losses. These excitations are analyzed microscopically with theoretical calculations using a 22-orbital model derived from first-principles electronic structure calculation. Based on the agreement with the experiment, the RIXS features are assigned to Fe-$d$ orbital excitations which, at low energies, are accompanied by spin flipping and dominated by Fe $d_{yz}$ and $d_{xz}$ orbital characters. Furthermore, our calculations suggest dispersive momentum dependence of the RIXS excitations below 0.5 eV, and predict remarkable splitting and merging of the lower-energy excitations in momentum space. Those excitations, which were not observed in the present experiment, highlight the potential of RIXS with an improved energy resolution to unravel new details of the electronic structure of the iron-based superconductors.
Resonant inelastic x-ray scattering (RIXS) is an extremely valuable tool for the study of elementary, including magnetic, excitations in matter. Latest developments of this technique mostly aimed at improving the energy resolution and performing polarization analysis of the scattered radiation, with a great impact on the interpretation and applicability of RIXS. Instead, this article focuses on the sample environment and presents a setup for high-pressure low-temperature RIXS measurements of low-energy excitations. The feasibility of these experiments is proved by probing the magnetic excitations of the bilayer iridate Sr$_3$Ir$_2$O$_7$ at pressures up to 12 GPa.
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