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Quantitative study of valence and configuration interaction parameters of the Kondo semiconductors CeM2Al10 (M = Ru, Os and Fe) by means of bulk-sensitive hard x-ray photoelectron spectroscopy

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 Added by Fabio Strigari
 Publication date 2014
  fields Physics
and research's language is English




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The occupancy of the 4f^n contributions in the Kondo semiconductors CeM2Al10(M = Ru, Os and Fe) has been quantitatively determined by means of bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) on the Ce 3d core levels. Combining a configuration interaction scheme with full multiplet calculations allowed to accurately describe the HAXPES data despite the presence of strong plasmon excitations in the spectra. The configuration interaction parameters obtained from this analysis -- in particular the hybridization strength V_eff and the effective f binding energy Delta_f -- indicate a slightly stronger exchange interaction in CeOs2Al10 compared to CeRu2Al10, and a significant increase in CeFe2Al10. This verifies the coexistence of a substantial amount of Kondo screening with magnetic order and places the entire CeM2Al10 family in the region of strong exchange interactions.



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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.
Bulk sensitive hard x-ray photoelectron spectroscopy data of the Ce 3$p$ core level of CeRu$_4$Sn$_6$ are presented. Using a combination of full multiplet and configuration iteration model we were able to obtain an accurate lineshape analysis of the data, thereby taking into account correlations for the strong plasmon intensities. We conclude that CeRu$_4$Sn$_6$ is a moderately mixed valence compound with a weight of 8% for the Ce $f^0$ configuration in the ground state.
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