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Yb Valence Change in (Ce,Yb)CoIn5 from spectroscopy and bulk properties

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 Added by Lenart Dudy
 Publication date 2013
  fields Physics
and research's language is English




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The electronic structure of (Ce,Yb)CoIn5 has been studied by a combination of photoemission, x-ray absorption and bulk property measurements. Previous findings of a Ce valence near 3+ for all x and of an Yb valence near 2.3+ for x>0.3 were confirmed. One new result of this study is that the Yb valence for x<0.2 increases rapidly with decreasing x from 2.3+ toward 3+, which correlates well with de Haas van Alphen results showing a change of Fermi surface around x=0.2. Another new result is the direct observation by angle resolved photoemission Fermi surface maps of about 50% cross sectional area reductions of the alpha- and beta-sheets for x=1 compared to x=0, and a smaller, essentially proportionate, size change of the alpha-sheet for x=0.2. These changes are found to be in good general agreement with expectations from simple electron counting. The implications of these results for the unusual robustness of superconductivity and Kondo coherence with increasing x in this alloy system are discussed.



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We investigated the onset of the many-body coherence in the f-orbital single crystalline alloys Ce(1-x)Yb(x)CoIn5 through thermodynamic and magneto-transport measurements. Our study shows the evolution of the many-body electronic state as the Kondo lattice of Ce moments is transformed into an array of Ce impurities. Specifically, we observe a smooth crossover from the predominantly localized Ce moment regime to the predominantly itinerant Yb f-electronic states regime for about 50% of Yb doping. Our analysis of the residual resistivity data unveils the presence of correlations between Yb ions, while from our analysis of specific heat data we conclude that for 0.65<x<0.775, ytterbium f-electrons strongly interact with the conduction electrons while the Ce moments remain completely decoupled. The sub-linear temperature dependence of resistivity across the whole range of Yb concentrations suggest the presence of a nontrivial scattering mechanism for the conduction electrons.
In this paper we review some of our recent experimental and theoretical results on transport and thermodynamic properties of heavy-fermion alloys Ce(1-x)Yb(x)CoIn5. Charge transport measurements under magnetic field and pressure on these single crystalline alloys revealed that: (i) relatively small Yb substitution suppresses the field induced quantum critical point, with a complete suppression for nominal Yb doping x>0.20; (ii) the superconducting transition temperature Tc and Kondo lattice coherence temperature T* decrease with x, yet they remain finite over the wide range of Yb concentrations; (iii) both Tc and T* increase with pressure; (iv) there are two contributions to resistivity, which show different temperature and pressure dependences, implying that both heavy and light quasiparticles contribute to inelastic scattering. We also analyzed theoretically the pressure dependence of both T* and Tc within the composite pairing theory. In the purely static limit, when we ignore the lattice dynamics, we find that the composite pairing mechanism necessarily causes opposite behaviors of T* and Tc with pressure: if T* grows with pressure, Tc must decrease with pressure and vice versa.
Here we present our experimental and theoretical study of the effects of pressure on the transport properties of the heavy-fermion alloy Ce(1-x)Yb(x)CoIn5 with x~0.07. We specifically choose this value of ytterbium concentration because the magnetic-field-induced quantum critical point, which separates the antiferromagnetic and paramagnetic states at zero temperature, approaches zero, as has been established in previous studies. Our measurements show that pressure further suppresses quantum fluctuations in this alloy, just as it does in the parent compound CeCoIn5. In contrast, the square-root temperature dependent part of resistivity remains insensitive to pressure, indicating that the heavy-quasiparticles are not involved in the scattering processes leading to such a temperature dependent resistivity. We demonstrate that the growth of the coherence temperature with pressure, as well as the decrease of the residual resistivity, can be accurately described by employing the coherent potential approximation for a disordered Kondo lattice.
A diffraction experiment using a high energy x-ray was carried out on YbInCu4. Below the Yb valence transition temperature, the splitting of Bragg peaks was detected in higher-order reflections. No superlattice reflections accompanying the valence ordering were found below the transition temperature. These experimental findings indicate that a structural change from a cubic structure to a tetragonal structure without valence ordering occurs at the transition temperature. Such a structural change free from any valence ordering is difficult to understand only in terms of Yb valence degrees of freedom. This means that the structural change may be related to electronic symmetries such as quadrupolar degrees of freedom as well as the change in Yb valence.
We study the electronic structure of Tsai-type cluster-based quasicrystalline approximants, Au$_{64}$Ge$_{22}$Yb$_{14}$ (AGY-I), Au$_{63.5}$Ge$_{20.5}$Yb$_{16}$ (AGY-II), and Zn$_{85.4}$Yb$_{14.6}$ (Zn-Yb), by means of photoemission spectroscopy. In the valence band hard x-ray photoemission spectra of AGY-II and Zn-Yb, we separately observe a fully occupied Yb 4$f$ state and a valence fluctuation derived Kondo resonance peak, reflecting two inequivalent Yb sites, a single Yb atom in the cluster center and its surrounding Yb icosahedron, respectively. The fully occupied 4$f$ signal is absent in AGY-I containing no Yb atom in the cluster center. The results provide direct evidence for a heterogeneous valence state in AGY-II and Zn-Yb.
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