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High-resolution Ce 3d-edge resonant photoemission study of CeNi_2

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 Added by Han-Jin Noh
 Publication date 1999
  fields Physics
and research's language is English




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Resonant photoemission (RPES) at the Ce 3d -> 4f threshold has been performed for alpha-like compound CeNi_2 with extremely high energy resolution (full width at half maximum < 0.2 eV) to obtain bulk-sensitive 4f spectral weight. The on-resonance spectrum shows a sharp resolution-limited peak near the Fermi energy which can be assigned to the tail of the Kondo resonance. However, the spin-orbit side band around 0.3 eV binding energy corresponding to the f_{7/2} peak is washed out, in contrast to the RPES spectrum at the Ce 3d -> 4f RPES threshold. This is interpreted as due to the different surface sensitivity, and the bulk-sensitive Ce 3d -> 4f RPES spectra are found to be consistent with other electron spectroscopy and low energy properties for alpha-like Ce-transition metal compounds, thus resolves controversy on the interpretation of Ce compound photoemission. The 4f spectral weight over the whole valence band can also be fitted fairly well with the Gunnarsson-Schoenhammer calculation of the single impurity Anderson model, although the detailed features show some dependence on the hybridization band shape and (possibly) Ce 5d emissions.



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The bulk-sensitive Ce 4$f$ spectral weights of various Ce compounds including CeFe$_2$, CeNi$_2$, and CeSi$_2$ were obtained with the resonant photoemission technique at the Ce 3d-edge. We found the lineshapes change significantly with the small change of the incident photon energy. Detailed analysis showed that this phenomenon results primarily from the Auger transition between different multiplet states of the Ce $underline{3d_{5/2}}4f^2$ (bar denotes a hole) electronic configuration in the intermediate state of the resonant process. This tells us that extra care should be taken for the choice of the resonant photon energy when extracting Ce 4$f$ spectral weights from the Ce 3$d$-edge resonant photoemission spectra. The absorption energy corresponding to the lowest multiplet structure of the Ce $underline{3d_{5/2}}4f^2$ configuration seems to be the logical choice.
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We present a high-resolution photoemission study on the strongly correlated Ce-compounds CeCu_6, CeCu_2Si_2, CeRu_2Si_2, CeNi_2Ge_2, and CeSi_2. Using a normalization procedure based on a division by the Fermi-Dirac distribution we get access to the spectral density of states up to an energy of 5 k_BT above the Fermi energy E_F. Thus we can resolve the Kondo resonance and the crystal field (CF) fine-structure for different temperatures above and around the Kondo temperature T_K. The CF peaks are identified with multiple Kondo resonances within the multiorbital Anderson impurity model. Our theoretical 4f spectra, calculated from an extended non-crossing approximation (NCA), describe consistently the observed photoemission features and their temperature dependence. By fitting the NCA spectra to the experimental data and extrapolating the former to low temperatures, T_K can be extracted quantitatively. The resulting values for T_K and the crystal field energies are in excellent agreement with the results from bulk sensitive measurements, e.g. inelastic neutron scattering.
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Resonant inverse photoemission spectra of Ni metal have been obtained across the Ni 3$p$ absorption edge. The intensity of Ni 3$d$ band just above Fermi edge shows asymmetric Fano-like resonance. Satellite structures are found at about 2.5 and 4.2 eV above Fermi edge, which show resonant enhancement at the absorption edge. The satellite structures are due to a many-body configuration interaction and confirms the existence of 3$d^8$ configuration in the ground state of Ni metal.
Spin- and angle-resolved resonant (Ce $4dto4f$) photoemission spectra of a monolayer Ce on Fe(110) reveal spin-dependent changes of the Fermi-level peak intensities. That indicate a spin-dependence of $4f$ hybridization and, thus, of $4f$ occupancy and local moment. The phenomenon is described in the framework of the periodic Anderson model by $4f$ electron hopping into the exchange split Fe 3d derived bands that form a spin-gap at the Fermi energy around the $bar{Gamma}$ point of the surface Brillouin zone.
We have performed a photoemission spectroscopy (PES) study of CeM2Al10 (M = Fe, Ru, and Os) to directly observe the electronic structure involved in the unusual magnetic ordering. Soft X-ray resonant (SXR) PES provides spectroscopic evidence of the hybridization between conduction and Ce 4f electrons (c-f hybridization) and the order of the hybridization strength (Ru < Os < Fe). High-resolution (HR) PES of CeRu2Al10 and CeOs2Al10, as compared with that of CeFe2Al10, identifies two structures that can be ascribed to structures induced by the c-f hybridization and the antiferromagnetic ordering, respectively. Although the c-f hybridization-induced structure is a depletion of the spectral intensity (pseudogap) around the Fermi level (EF) with an energy scale of 20-30 meV, the structure related to the antiferromagnetic ordering is observed as a shoulder at approximately 10-11 meV within the pseudogap. The energies of the shoulder structures of CeRu2Al10 and CeOs2Al10 are approximately half of the optical gap (20 meV), indicating that EF is located at the midpoint of the gap.
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