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Superconducting properties of Pr-based Filled skutterudite PrRu$_4$As$_{12}$

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 Added by Takahiro Namiki
 Publication date 2007
  fields Physics
and research's language is English




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We report on systematic study of superconducting characteristics and Pr crystalline-electric-field (CEF) levels of filled-skutterudite pra ($T_{rm c}$ = 2.33 K). The temperature dependences of the upper critical field $H_{rm c2}$ and the Ginzburg-Landau (Maki) parameter $kappa_2$ suggest an s-wave clean-limit superconductivity. The electronic specific heat coefficient $gamma sim 95$ mJ/K$^2$mol, being $sim 1.5$ times larger than that for lra, indicates $4f$-originating quasiparticle mass enhancement. Magnetic susceptibility $chi(T)$ indicates that the CEF ground state is a $Gamma_1$ singlet and a $Gamma_4^{(1)}$ triplet first excited state lies at $Delta_{rm CEF}sim 30$ K above. Systematic comparison among pos, prs, pra and La-based reference compounds suggests that inelastic exchange- and aspherical-charge-scatterings of conduction electrons from CEF-split $4f$ levels play an essential role for the quasiparticle mass enhancement and the value of $T_{rm c}$ in the Pr-based filled skutterudites.



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Comprehensive magnetic-field-orientation dependent studies of the susceptibility and de Haas-van Alphen effect have been carried out on single crystals of the filled skutterudites PrOs$_4$As$_{12}$ and LaOs$_4$As$_{12}$ using magnetic fields of up to 40~T. Several peaks are observed in the low-field susceptibility of PrOs$_4$As$_{12}$, corresponding to cascades of metamagnetic transitions separating the low-field antiferromagnetic and high-field paramagnetic metal (PMM) phases. The de Haas-van Alphen experiments show that the Fermi-surface topologies of PrOs$_4$As$_{12}$ in its PMM phase and LaOs$_4$As$_{12}$ are very similar. In addition, they are in reasonable agreement with the predictions of bandstructure calculations for LaOs$_4$As$_{12}$ on the PrOs$_4$As$_{12}$ lattice. Both observations suggest that the Pr 4$f$ electrons contribute little to the number of itinerant quasiparticles in the PMM phase. However, whilst the properties of LaOs$_4$As$_{12}$ suggest a conventional nonmagnetic Fermi liquid, the effects of direct exchange and electron correlations are detected in the PMM phase of PrOs$_4$As$_{12}$. For example, the quasiparticle effective masses in PrOs$_4$As$_{12}$ are found to decrease with increasing field, probably reflecting the gradual suppression of magnetic fluctuations associated with proximity to the low-temperature, low-field antiferromagnetic state.
76 - Y. Aoki , T. Namiki , T. Kanayama 2002
Rare 4f^2-based heavy-fermion behaviors have been revealed recently in Pr-based filled skutterudites PrFe4P12 and PrOs4Sb12. Recent studies on the thermal properties on both compounds are reported, putting emphasis on the field-induced ordered phase found in PrOs4Sb12.
Motivated by current research efforts towards exploring the interplay between magnetism and superconductivity in multiband electronic systems, we have investigated the effects of Eu substitution through thermodynamic measurements on the superconducting filled skutterudite alloys Pr$_{1-x}$Eu$_x$Pt$_4$Ge$_{12}$. An increase in Eu concentration leads to a suppression of the superconducting transition temperature consistent with an increase of magnetic entropy due to Eu local moments. While the low-temperature heat capacity anomaly is present over the whole doping range, we find that in alloys with $xleq0.5$ the Schottky peaks in the heat capacity in the superconducting state appear to be due to Zeeman splitting by an internal magnetic field. Our theoretical modeling suggests that this field is a result of the short-range antiferromagnetic correlations between the europium ions. For the samples with $x > 0.5$, the peaks in the heat capacity signal the onset of antiferromagnetic (AFM) ordering of the Eu moments.
Anomalous metal-insulator transition observed in filled skutterudite CeOs$_4$Sb$_{12}$ is investigated by constructing the effective tight-binding model with the Coulomb repulsion between f electrons. By using the mean field approximation, magnetic susceptibilities are calculated and the phase diagram is obtained. When the band structure has a semimetallic character with small electron and hole pockets at $Gamma$ and H points, a spin density wave transition with the ordering vector $mathbf{Q}=(1,0,0)$ occurs due to the nesting property of the Fermi surfaces. Magnetic field enhances this phase in accord with the experiments.
Superconductivity, magnetic order, and quadrupolar order have been investigated in the filled skutterudite system Pr$_{1-x}$Nd$_{x}$Os$_4$Sb$_{12}$ as a function of composition $x$ in magnetic fields up to 9 tesla and at temperatures between 50 mK and 10 K. Electrical resistivity measurements indicate that the high field ordered phase (HFOP), which has been identified with antiferroquadruoplar order, persists to $x$ $sim$ 0.5. The superconducting critical temperature $T_c$ of PrOs$_4$Sb$_{12}$ is depressed linearly with Nd concentration to $x$ $sim$ 0.55, whereas the Curie temperature $T_{FM}$ of NdOs$_4$Sb$_{12}$ is depressed linearly with Pr composition to ($1-x$) $sim$ 0.45. In the superconducting region, the upper critical field $H_{c2}(x,0)$ is depressed quadratically with $x$ in the range 0 $<$ $x$ $lesssim$ 0.3, exhibits a kink at $x$ $approx$ 0.3, and then decreases linearly with $x$ in the range 0.3 $lesssim$ $x$ $lesssim$ 0.6. The behavior of $H_{c2}(x,0)$ appears to be due to pair breaking caused by the applied magnetic field and the exhange field associated with the polarization of the Nd magnetic moments, in the superconducting state. From magnetic susceptibility measurements, the correlations between the Nd moments in the superconducting state appear to change from ferromagnetic in the range 0.3 $lesssim$ $x$ $lesssim$ 0.6 to antiferromagnetic in the range 0 $<$ $x$ $lesssim$ 0.3. Specific heat measurements on a sample with $x$ $=$ 0.45 indicate that magnetic order occurs in the superconducting state, as is also inferred from the depression of $H_{c2}(x,0)$ with $x$.
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