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Register a new userUncovering selective excitations using the resonant profile of indirect inelastic x-ray scattering in correlated materials: Observing two-magnon scattering and relation to the dynamical structure factor
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Resonant inelastic x-ray scattering (RIXS) is a spectroscopic technique which has been widely used to study various elementary excitations in correlated and other condensed matter systems. For strongly correlated materials, besides boosting the overall signal the dependence of the resonant profile on incident photon energy is still not fully understood. Previous endeavors in connecting indirect RIXS, such as Cu K-edge for example where scattering takes place only via the core-hole created as an intermediate state, with the charge dynamical structure factor S(q,omega) neglected complicated dependence on the intermediate state configuration. To resolve this issue, we performed an exact diagonalization study of the RIXS cross-section using the single-band Hubbard model by fully addressing the intermediate state contribution. Our results are relevant to indirect RIXS in correlated materials, such as high Tc cuprates. We demonstrate that RIXS spectra can be reduced to S(q,omega) when there is no screening channel for the core-hole potential in the intermediate state. We also show that two-magnon excitations are highlighted at the resonant photon energy when the core-hole potential in the corresponding intermediate state is poorly screened. Our results demonstrate that different elementary excitations can be emphasized at different intermediate states, such that selecting the exact incident energy is critical when trying to capture a particular elementary excitation.
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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.
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.
We have used high-resolution resonant inelastic x-ray scattering (RIXS) to study a thin film of NdNiO$_3$, a compound whose unusual spin- and bond-ordered electronic ground state has been of long-standing interest. Below the magnetic ordering temperature, we observe well-defined collective magnon excitations along different high-symmetry directions in momentum space. The magnetic spectra depend strongly on the incident photon energy, which we attribute to RIXS coupling to different local electronic configurations of the expanded and compressed NiO$_6$ octahedra in the bond-ordered state. Both the noncollinear magnetic ground state and the observed site-dependent magnon excitations are well described by a model that assumes strong competition between the antiferromagnetic superexchange and ferromagnetic double-exchange interactions. Our study provides direct insight into the magnetic dynamics and exchange interactions of the rare-earth nickelates, and demonstrates that RIXS can serve as a site-selective probe of magnetism in these and other materials.
We report a Cu K-edge resonant inelastic x-ray scattering (RIXS) study of high-Tc cuprates. Momentum-resolved charge excitations in the CuO2 plane are examined from parent Mott insulators to carrier-doped superconductors. The Mott gap excitation in undoped insulators is found to commonly show a larger dispersion along the [pi,pi] direction than the [pi,0] direction. On the other hand, the resonance condition displays material dependence. Upon hole doping, the dispersion of the Mott gap excitation becomes weaker and an intraband excitation appears as a continuum intensity below the gap at the same time. In the case of electron doping, the Mott gap excitation is prominent at the zone center and a dispersive intraband excitation is observed at finite momentum transfer.
To fully capitalize on the potential and versatility of resonant inelastic x-ray scattering (RIXS), it is essential to develop the capability to interpret different RIXS contributions through calculations, including the dependence on momentum transfer, from first-principles for correlated materials. Toward that objective, we present new methodology for calculating the full RIXS response of a correlated metal in an unbiased fashion. Through comparison of measurements and calculations that tune the incident photon energy over a wide portion of the Fe L$_3$ absorption resonance of the example material BaFe$_2$As$_2$, we show that the RIXS response in BaFe$_2$As$_2$ is dominated by the direct channel contribution, including the Raman-like response below threshold, which we explain as a consequence of the finite core-hole lifetime broadening. Calculations are initially performed within the first-principles Bethe-Salpeter framework, which we then significantly improve by convolution with an effective spectral function for the intermediate-state excitation. We construct this spectral function, also from first-principles, by employing the cumulant expansion of the Greens function and performing a real-time time dependent density functional theory calculation of the response of the electronic system to the perturbation of the intermediate-state excitation. Importantly, this allows us to evaluate the indirect RIXS response from first-principles, accounting for the full periodicity of the crystal structure and with dependence on the momentum transfer.
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