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Detection of Acoustic Plasmons in Hole-Doped Lanthanum and Bismuth Cuprate Superconductors Using Resonant Inelastic X-Ray Scattering

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 Added by Ke-Jin Zhou
 Publication date 2020
  fields Physics
and research's language is English




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High Tc superconductors show a rich variety of phases associated with their charge degrees of freedom. Valence charges can give rise to charge ordering or acoustic plasmons in these layered cuprate superconductors. While charge ordering has been observed for both hole- and electron-doped cuprates, acoustic plasmons have only been found in electron-doped materials. Here, we use resonant inelastic X-ray scattering (RIXS) to observe the presence of acoustic plasmons in two families of hole-doped cuprate superconductors [La2-xSrxCuO4 (LSCO) and Bi2Sr1.6La0.4CuO6+d (Bi2201)], crucially completing the picture. Interestingly, in contrast to the quasi-static charge ordering which manifests at both Cu and O sites, the observed acoustic plasmons are predominantly associated with the O sites, revealing a unique dichotomy in the behaviour of valence charges in hole-doped cuprates.



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The superconductivity of cuprates, which has been a mystery ever since its discovery decades ago, is created through doping electrons or holes into a Mott insulator. There, however, exists an inherent electron-hole asymmetry in cuprates. The layered crystal structures of cuprates enable collective charge excitations fundamentally different from those of three-dimensional metals, i.e., acoustic plasmons. Acoustic plasmons have been recently observed in electron-doped cuprates by resonant inelastic X-ray scattering (RIXS); in contrast, there is no evidence for acoustic plasmons in hole-doped cuprates, despite extensive measurements. This contrast led us to investigate whether the doped holes in cuprates La$_{2-x}$Sr$_x$CuO$_4$ are conducting carriers or are too incoherent to induce collective charge excitation. Here we present momentum-resolved RIXS measurements and calculations of collective charge response via the loss function to reconcile the aforementioned issues. Our results provide unprecedented spectroscopic evidence for the acoustic plasmons and long sought conducting p holes in hole-doped cuprates.
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.
The ladder compound Sr$_{14}$Cu$_{24}$O$_{41}$ is of interest both as a quasi-one-dimensional analog of the superconducting cuprates and as a superconductor in its own right when Sr is substituted by Ca. In order to model resonant inelastic x-ray scattering (RIXS) spectra for this compound, we investigate the simpler SrCu$_{2}$O$_{3}$ system in which the crystal structure contains very similar ladder planes. We approximate the LDA dispersion of SrCu$_{2}$O$_{3}$ by a Cu only two-band tight-binding model. Strong correlation effects are incorporated by assuming an anti-ferromagnetic ground state. The available angle-resolved photoemission (ARPES) and RIXS data on the ladder compound are found to be in reasonable accord with our theoretical predictions.
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.
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