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Suppression of Nonmagnetic Insulating State by Application of Pressure in Mineral Tetrahedrite Cu$_{12}$Sb$_{4}$S$_{13}$

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 Added by Shunsaku Kitagawa
 Publication date 2015
  fields Physics
and research's language is English




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The mineral tetrahedrite Cu$_{12}$Sb$_{4}$S$_{13}$ exhibits a first-order metal--insulator transition (MIT) at $T_{rm MI}$ = 85 K and ambient pressure. We measured the $^{63}$Cu-NMR at ambient pressure and the resistivity and magnetic susceptibility at high pressures. $^{63}$Cu-NMR results indicate a nonmagnetic insulating ground state in this compound. The MIT is monotonically suppressed by pressure and disappears at $sim1.0$ GPa. Two other anomalies are observed in the resistivity measurements, and the pressure -- temperature phase diagram of Cu$_{12}$Sb$_{4}$S$_{13}$ is constructed.



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We have studied the pressure effect on the rattling of tetrahedrite Cu$_{10}$Zn$_{2}$Sb$_{4}$S$_{13,}$(CZSS) and type-I clathrate Ba$_{8}$Ga$_{16}$Sn$_{30,}$(BGS) by specific heat and x-ray diffraction measurements. By applying pressure $P$, the rattling energy for CZSS initially decreases and steeply increases for $P$ $textgreater$ $1$ GPa. By contrast, the energy for BGS increases monotonically with $P$ up to 6.5 GPa. An analysis of the pressure dependent specific heat and x-ray diffraction indicates that the out-of-plane rattling of the Cu atoms in the S$_{3}$ triangle of CZSS originates from the chemical pressure, unlike the rattling of the Ba ions among off-center sites in an oversized cage of BGS. The rattling in CZSS ceases upon further increasing $P$ above 2 GPa, suggesting that Cu atoms escape away from the S$_{3}$ triangle plane.
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.
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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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