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A new heavy fermion superconductor: the filled skutterudite compound PrOs$_4$Sb$_{12}$

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 Added by Neil Frederick
 Publication date 2003
  fields Physics
and research's language is English




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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.



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Thermal conductivity measurements were performed on single crystal samples of the superconducting filled skutterudite compounds PrOs$_4$Sb$_{12}$ and PrRu$_4$Sb$_{12}$ both as a function of temperature and magnetic field applied perpendicular to the heat current. In zero magnetic field, the low temperature electronic thermal conductivity of PrRu$_4$Sb$_{12}$ is vanishingly small, consistent with a fully-gapped Fermi surface. For PrOs$_4$Sb$_{12}$, however, we find clear evidence for residual electronic conduction as the temperature tends to zero Kelvin which is consistent with the presence of nodes in the superconducting energy gap. The field dependence of the electronic conductivity for both compounds shows a rapid rise immediately above H$_{c1}$ and significant structure over the entire vortex state. In the fully gapped superconductor PrRu$_4$Sb$_{12}$, this is interpreted in terms of multi-band effects. In PrOs$_4$Sb$_{12}$, we consider the Doppler shift of nodal quasiparticles at low fields and multiband effects at higher fields.
We present polar Kerr effect measurements of the filled skutterudite superconductor PrOs$_4$Sb$_{12}$. Simultaneous AC susceptibility measurements allow us to observe the superconducting transition under the influence of heating from the optical beam. A nonzero Kerr angle $theta_K$ develops below the superconducting transition, saturating at $sim 300$ nrad at low temperatures. This result is repeated across several measurements of multiple samples. By extrapolating the measured $theta_K(T)$ to zero optical power, we are able to show that the Kerr angle onset temperature in one set of measurements is consistent with the transition to the B phase at $T_{C2}$. We discuss the possible explanations for this result and its impact on the understanding of multi-phase and inhomogeneous superconductivity in PrOs$_4$Sb$_{12}$.
We have investigated the de Haas-van Alphen effect in the Pr-based heavy fermion superconductor PrOs$_4$Sb$_{12}$.The topology of Fermi surface is close to the reference compound LaOs$_4$Sb$_{12}$ and well explained by the band structure calculation based on the FLAPW-LDA+U method, where the 4{it f} electrons are localized. We have confirmed a highly enhanced cyclotron effective mass 2.4$sim7.6m_{rm 0}$ which is apparently large compared to the usual Pr-based compounds.
We have measured the electrical resistivity, thermoelectric power, Hall coefficient, and magnetoresistance (MR) on single crystals of PrOs$_{4}$Sb$_{12}$, LaOs$_{4}$Sb$_{12}$ and NdOs$_{4}$Sb$_{12}$. All the transport properties in PrOs$_{4}$Sb$_{12}$ are similar to those in LaOs$_{4}$Sb$_{12}$ and NdOs$_{4}$Sb$_{12}$ at high temperatures, indicating the localized character of 4$f$-electrons. The transverse MR both in LaOs$_{4}$Sb$_{12}$ and PrOs$_{4}$Sb$_{12}$ tends to saturate for wide field directions, indicating these compounds to be uncompensated metals with no open orbit. We have determined the phase diagram of the field induced ordered phase by the MR measurement for all the principle field directions, which indicates an unambiguous evidence for the $Gamma_{rm 1}$ singlet crystalline electric field ground state.
We report the electronic and superconducting properties in the Pr-based filled-skutterudite superconductor PrRu$_4$Sb$_{12}$ with $T_c = 1.3$ K via the measurements of nuclear-quadrupole-resonance (NQR) frequency $ u_Q$ and nuclear-spin-lattice-relaxation time $T_1$ of Sb nuclei. The temperature dependence of $ u_Q$ has revealed the energy scheme of Pr$^{3+}$ crystal electric field (CEF) that is consistent with an energy separation $Delta_{CEF}sim 70$K between the ground state and the first-excited state. In the normal state, the Korringa relation of $(1/T_1T)_{Pr}$=const. is valid, with [$(1/T_{1}T$)$_{Pr}$/$(1/T_{1}T$)$_{La}$]$^{1/2}$ $sim$ 1.44 where $(1/T_1T)_{La}$ is for LaRu$_4$Sb$_{12}$. These results are understood in terms of a conventional Fermi liquid picture in which the Pr-$4f^2$ state derives neither magnetic nor quadrupolar degrees of freedom at low temperatures. In the superconducting state, $1/T_1$ shows a distinct coherence peak just below $T_c$, followed by an exponential decrease with a value of 2$Delta/k_{B}T_{c}$ = 3.1. These results demonstrate that PrRu$_4$Sb$_{12}$ is a typical weak-coupling s-wave superconductor, in strong contrast with the heavy-fermion superconductor PrOs$_4$Sb$_{12}$ that is in an unconventional strong coupling regime. The present study on PrRu$_4$Sb$_{12}$ highlights that the Pr-$4f^2$derived non-magnetic doublet plays a key role in the unconventional electronic and superconducting properties in PrOs$_4$Sb$_{12}$.
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