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Direct Observation of Quadrupolar Excitons in the Heavy-Fermion Superconductor PrOs$_{4}$Sb$_{12}$

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 Added by Keitaro Kuwahara
 Publication date 2005
  fields Physics
and research's language is English




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We report inelastic neutron scattering experiments performed to investigate the low energy magnetic excitations on single crystals of the heavy-fermion superconductor PrOs$_{4}$Sb$_{12}$. The observed excitation clearly softens at a wave vector Q = (1,0,0), which is the same as the modulation vector of the field-induced antiferro-quadrupolar ordering, and its intensity at Q = (1,0,0) is smaller than that around the zone center. This result directly evidences that this excitonic behavior is derived mainly from nonmagnetic quadrupolar interactions. Furthermore, the narrowing of the linewidths of the excitations below the superconducting transition temperature indicates the close connection between the superconductivity and the excitons.



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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 have investigated the electrical resistivity of the heavy fermion superconductor PrOs$_{4}$Sb$_{12}$ in the mixed state. We found unusual double minima in the flux-flow resistivity as a function of magnetic field below the upper critical field for the first time, indicating double peaks in the pinning force density ($F_{rm P}$). Estimated $F_{rm P}$ at the peak exhibits apparent dependence on applied field direction; composed of two-fold and four-fold symmetries mimicking the reported angular dependence of thermal conductivity ($kappa$). The result is discussed in correlation with the double step superconducting (SC) transition in the specific heat and the multiple SC-phases inferred from the angular dependence of $kappa$.
We report $^{121,123}$Sb nuclear quadrupole resonance (NQR) measurements in the filled-skutterudite superconductor PrOs$_4$Sb$_{12}$ in the temperature range of 0.05-30 K. The electric field gradients (EFG), $V_{zz}$ and $V_{xx}-V_{yy}$, at the Sb site exhibit unusual temperature dependence below 30 K. To explain these features, we discuss the coupling between the Sb nuclear quadrupole moment and Pr $4f^2$-derived multipole moments. The observed $T$ dependence of EFG is well explained by the CEF quasi-quartet consisted of $Gamma_1$ singlet and $Gamma_4^{(2)}$ triplet states in the cubic point group $T_h$. These results, in turn, are indicative of the importance of the coupling between the $^{121,123}$Sb quadrupole moments and the hexadecapole moment caused by the quasi-quartet.
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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