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Thermoelectricity of EuCu{2}(Ge{1-x}Si{x}){2} intermetallics

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 Added by V. Zlatic
 Publication date 2005
  fields Physics
and research's language is English
 Authors Veljko Zlatic




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The evolution of the thermopower EuCu{2}(Ge{1-x}Si{x}){2} intermetallics, which is induced by the Si-Ge substitution, is explained by the Kondo scattering of conduction electrons on the Eu ions which fluctuate between the magnetic 2+ and non-magnetic 3+ Hunds rule configurations. The Si-Ge substitution is equivalent to chemical pressure which modifies the coupling and the relative occupation of the {it f} and conduction states.



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In mixed-valence or heavy-fermion systems, the hybridization between local $f$ orbitals and conduction band states can cause the suppression of long-range magnetic order, which competes with strong spin fluctuations. Ce- and Yb-based systems have been found to exhibit fascinating physical properties (heavy-fermion superconductivity, non-Fermi-liquid states, etc.) when tuned to the vicinity of magnetic quantum critical points by use of various external control parameters (temperature, magnetic field, chemical composition). Recently, similar effects (mixed-valence, Kondo fluctuations, heavy Fermi liquid) have been reported to exist in some Eu-based compounds. Unlike Ce (Yb), Eu has a multiple electron (hole) occupancy of its $4f$ shell, and the magnetic Eu$^{2+}$ state ($4f^7$) has no orbital component in the usual $LS$ coupling scheme, which can lead to a quite different and interesting physics. In the EuCu$_{2}$(Si$_{x}$Ge$_{1-x}$)$_{2}$ series, where the valence can be tuned by varying the Si/Ge ratio, it has been reported that a significant valence fluctuation can exist even in the magnetic order regime. This paper presents a detailed study of the latter material using different microscopic probes (XANES, Mossbauer spectroscopy, elastic and inelastic neutron scattering), in which the composition dependence of the magnetic order and dynamics across the series is traced back to the change in the Eu valence state. In particular, the results support the persistence of valence fluctuations into the antiferromagnetic state over a sizable composition range below the critical Si concentration $x_c approx 0.65$. The sequence of magnetic ground states in the series is shown to reflect the evolution of the magnetic spectral response.
The magnetic properties of polycrystalline Tb(Co_{x}Ni_{1-x})_{2}B_{2}C (x=0.2,0.4,0.6,0.8) samples were probed by magnetization, specific heat, ac susceptibility, and resistivity techniques. For x{ eq}0.4, the obtained curves are consistent with the features expected for the corresponding magnetic modes, namely k_{1}=(0.55,0,0) at x=0; k_{2}=([nicefrac] icefrac{1}{2}</LaTeX>,0,[nicefrac]<LaTeX> icefrac{1}{2}) at x= 0.2; k_{3}=(0,0,[nicefrac] icefrac{1}{3}) at x= 0.6, and k_{4}=(0,0,0) at x= 0.8 and 1. For x=0.4, even though the neutron diffraction indicates a k_{2} mode, but with a reduced magnetic moment, the magnetization, the ac susceptibility, and resistivity indicate two magnetic events; furthermore, deviation from Curie-Weiss behavior is observed below 150 K for this sample. These features, together with the evolution of both magnetic moment and critical temperature, are attributed to an interplay between competing magnetic couplings; for the particular x=0.4 case, additional factors such as crystalline electric field effects may be in operation.
We report specific heat and neutron scattering experiments performed on the system Ce$_{1-x}$La$_{x}$Ru$_{2}$Si$_{2}$ on the magnetic side of its quantum critical phase diagram. The Kondo temperature does not vanish at the quantum phase transition and elastic scattering indicates a gradual localisation of the magnetism when $x$ increases in the ordered phase.
228 - T. Okane , T. Ohkochi , Y. Takeda 2009
Angle-resolved photoelectron spectroscopy in the Ce 3d-4f excitation region was measured for the paramagnetic state of CeRu2Si2, CeRu2(Si0.82Ge0.18)2, and LaRu2Si2 to investigate the changes of the 4$f$ electron Fermi surfaces around the quantum critical point. While the difference of the Fermi surfaces between CeRu2Si2 and LaRu2Si2 was experimentally confirmed, a strong 4f-electron character was observed in the band structures and the Fermi surfaces of CeRu2Si2 and CeRu2(Si0.82Ge0.18)2, consequently indicating a delocalized nature of the 4$f$ electrons in both compounds. The absence of Fermi surface reconstruction across the critical composition suggests that SDW quantum criticality is more appropriate than local quantum criticality in CeRu2(Si[1-x]Ge[x])2.
We report the detailed electronic structure of a hole-doped delafossite oxide CuCr_{1-x}Mg_{x}O_{2} (0 <= x <= 0.03) studied by photoemission spectroscopy (PES), soft x-ray absorption spectroscopy (XAS), and band-structure calculations within the local-density approximation +U (LDA+U) scheme. Cr/Cu 3p-3d resonant PES reveals that the near-Fermi-level leading structure has primarily the Cr 3d character with a minor contribution from the Cu 3d through Cu 3d-O 2p-Cr 3d hybridization, having good agreement with the band-structure calculations. This indicates that a doped hole will have primarily the Cr 3d character. Cr 2p PES and L-edge XAS spectra exhibit typical Cr^{3+} features for all x, while the Cu L-edge XAS spectra exhibited a systematic change with x. This indicates now that the Cu valence is monovalent at x=0 and the doped hole should have Cu 3d character. Nevertheless, we surprisingly observed two types of charge-transfer satellites that should be attributed to Cu^{+} (3d^{10}) and Cu^{2+} (3d^{9}) like initial states in Cu 2p-3d resonant PES spectrum for at x=0, while Cu 2p PES spectra with no doubt shows the Cu^{+} character even for the lightly doped samples. We propose that these contradictory results can be understood by introducing no only the Cu 4s state, but also finite Cu 3d,4s-Cr 3d charge transfer via O 2p states in the ground-state electronic configuration.
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