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Multiple ordered phases in the filled skutterudite compound PrOs$_{4}$As$_{12}$

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 Added by William Yuhasz
 Publication date 2005
  fields Physics
and research's language is English




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Magnetization, specific heat, and electrical resistivity measurements were made on single crystals of the filled skutterudite compound PrOs$_{4}$As$_{12}$. Specific heat measurements indicate an electronic specific heat coefficient $gamma$ $sim 50-200$ mJ/mol K$^{2}$ at temperatures 10 K $leq T leq 18$ K, and $sim 1$ J/mol K$^{2}$ for $T leq 1.6$ K. Magnetization, specific heat, and electrical resistivity measurements reveal the presence of two, or possibly three, ordered phases at temperatures below $sim 2.3$ K and in fields below $sim 3$ T. The low temperature phase displays antiferromagnetic characteristics, while the nature of the ordering in the other phase(s) has yet to be determined.



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X-ray diffraction, electrical resistivity, magnetization, specific heat, and thermoelectric power measurements are presented for single crystals of the new filled skutterudite compound {CeOsAs}, which reveal phenomena that are associated with f - electron - conduction electron hybridization. Valence fluctuations or Kondo behavior dominates the physics down to $T$ $sim$ 135 K. The correlated electron behavior is manifested at low temperatures as a hybridization gap insulating state. The small energy gap $Delta$$_1$/k$_B$ $sim$ 73 K, taken from fits to electrical resistivity data, correlates with the evolution of a weakly magnetic or nonmagnetic ground state, which is evident in the magnetization data below a coherence temperature $T$$_{coh}$ $sim$ 45 K. Additionally, the low temperature electronic specific heat coefficient is small, $gamma$ $sim$ 19 mJ/mol K$^2$. Some results for the nonmagnetic analogue compound {LaOsAs} are also presented for comparison purposes.
The filled skutterudite compound PrOsSb{} exhibits superconductivity below a critical temperature $T_mathrm{c} = 1.85$ K that develops out of a nonmagnetic heavy Fermi liquid with an effective mass $m^{*} approx 50 m_mathrm{e}$, where $m_mathrm{e}$ is the free electron mass. Analysis of magnetic susceptibility, specific heat, electrical resistivity and inelastic neutron scattering measurements within the context of a cubic crystalline electric field yields a Pr$^{3+}$ energy level scheme that consists of a $Gamma_{3}$ nonmagnetic doublet ground state that carries an electric quadrupole moment, a low lying $Gamma_{5}$ triplet excited state at $sim 10$ K, and $Gamma_{4}$ triplet and $Gamma_{1}$ singlet excited states at much higher temperatures. The superconducting state appears to be unconventional and to consist of two distinct superconducting phases. An ordered phase of magnetic or quadrupolar origin occurs at high fields and low temperatures, suggesting that the superconductivity may occur in the vicinity of a magnetic or electric quadrupolar quantum critical point.
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.
Electrical resistivity $rho$, specific heat C, and magnetic susceptibility $chi$ measurements made on the filled skutterudite CeRu_4As_{12} reveal non-Fermi liquid (NFL) T - dependences at low T, i.e., $rho$(T) $sim$ T^{1.4} and weak power law or logarithmic divergences in C(T)/T and $chi$(T). Measurements also show that the T - dependence of the thermoelectric power S(T) deviates from that seen in other Ce systems. The NFL behavior appears to be associated with fluctuations of the Ce valence between 3^+ and 4^+ rather than a typical Kondo lattice scenario that would be appropriate for an integral Ce valence of 3^+.
325 - T. Namiki , Y. Aoki , H. Sato 2007
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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