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Register a new userMapping the Electronic Structure of Warm Dense Nickel via Resonant Inelastic X-ray Scattering
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The development of high-brightness free-electron lasers (FEL) has revolutionised our ability to create and study matter in the high-energy-density (HED) regime. Current diagnostic techniques have been very successful in yielding information on fundamental thermodynamic plasma properties, but provide only limited or indirect information on the detailed quantum structure of these systems, and on how it is affected by ionization dynamics. Here we show how the electronic structure of solid-density nickel, heated to temperatures of 10s of eV on femtosecond timescales, can be studied by resonant (Raman) inelastic x-ray scattering (RIXS) using the Linac Coherent Light Source FEL. We present single-shot measurements of the valence density of states in the x-ray-heated transient system, and extract simultaneously electron temperatures, ionization, and ionization potential energies. The RIXS spectrum provides a wealth of information on the valence structure of the HED system that goes beyond what can be extracted from x-ray absorption or emission spectroscopy alone.
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We report a comprehensive Cu $K$-edge RIXS investigation of $rm La_{2-x}Sr_xCuO_4$ (LSCO) for 0$leq$x$leq$0.35, stripe-ordered $rm La_{1.875}Ba_{0.125}CuO_4$ (LBCO), and $rm La_{2}Cu_{0.96}Ni_{0.04}O_4$ (LCNO) crystals. The RIXS spectra measured at three high-symmetry momentum transfer (textbf{q}) positions are compared as a function of doping and for the different dopants. The spectra in the energy range 1-6 eV can be described with three broad peaks, which evolve systematically with increased doping. The most systematic trend was observed for textbf{q}=($pi$, 0) corresponding to the zone boundary. As hole doping increased, the spectral weight transfer from high energies to low energies is nearly linear with emph{x} at this textbf{q}. We interpret the peaks as interband transitions in the context of existing band models for this system, assigning them to Zhang-Rice band$rightarrow$upper Hubbard band, lower-lying band$rightarrow$upper Hubbard band, and lower-lying band$rightarrow$Zhang-Rice band transitions. The spectrum of stripe-ordered LBCO was also measured, and found to be identical to the correspondingly doped LSCO, except for a relative enhancement of the near-infrared peak intensity around 1.5-1.7 eV. The temperature dependence of this near-infrared peak in LBCO was more pronounced than for other parts of the spectrum, continuously decreasing in intensity as the temperature was raised from 25 K to 300 K. Finally, we find that 4% Ni substitution in the Cu site has a similar effect on the spectra as does Sr substitution in the La site.
Recent calculations [Nilsen et al. arXiv:1212.5972] predict that contributions to the scattered photon spectrum from 3s and 3p bound states in chromium (Z=24) at metallic density and T=12 eV resonate below the respective bound-state thresholds. These resonances are shown to be closely related to continuum lowering, where 3d bound states in the free atom dissolve into a resonant l=2 partial wave in the continuum. The resulting d-state resonance dominates contributions to the bound-free dynamic structure function, leading to the predicted resonances in the scattered X-ray spectrum. Similar resonant features are shown to occur in all elements in the periodic table between Ca and Mn (20 <= Z <= 25).
A scheme for analyzing Thomson scattering of x-rays by warm dense matter, based on the average-atom model, is developed. Emphasis is given to x-ray scattering by bound electrons. Contributions to the scattered x-ray spectrum from elastic scattering by electrons moving with the ions and from inelastic scattering by free and bound electrons are evaluated using parameters (chemical potential, average ionic charge, free electron density, bound and continuum wave functions, and occupation numbers) taken from the average-atom model. The resulting scheme provides a relatively simple diagnostic for use in connection with x-ray scattering measurements. Applications are given to dense hydrogen, beryllium, aluminum, titanium, and tin plasmas. At high momentum transfer, contributions from inelastic scattering by bound electrons are dominant features of the scattered x-ray spectrum for aluminum, titanium, and tin.
Results of resonant inelastic X-ray scattering (RIXS) measurements at Fe L-edges and electronic structure calculations of LiFeAs and NaFeAs are presented. Both experiment and theory show that in the vicinity of the Fermi energy, the density of states is dominated by contributions from Fe 3d-states. The comparison of Fe L2,3 non-resonant and resonant (excited at L2-threshold) X-ray emission spectra with spectra of LaOFeAs and CaFe2As2 show a great similarity in energy and I(L2)/I(L3) intensity ratio. The I(L2)/I(L3) intensity ratio of all FeAs-based superconductors is found to be more similar to metallic Fe than to correlated FeO. Basing on these measurements we conclude that iron-based superconductors are weakly or moderately correlated systems.
Topology is a central notion in the classification of band insulators and characterization of entangled many-body quantum states. In some cases, it manifests as quantized observables such as quantum Hall conductance. However, being inherently a global property depending on the entirety of the system, its direct measurement has remained elusive to local experimental probes in many cases. Here, we demonstrate that some topological band indices can be probed by resonant inelastic x-ray scattering. Specifically, for the paradigmatic Su-Schrieffer-Heeger and quadrupolar insulator models, we show that non-trivial band topology leads to distinct scattering intensity at particular momentum and energy. Our result establishes an incisive bulk probe for the measurement of band topology.
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