Simultaneous Superconducting and Antiferroquadrupolar Transitions in PrRh2_{2}Zn20_{20}

Superconducting and antiferroquadrupolar (AFQ) transitions in a Pr-based compound PrRh2Zn20 have been found to occur simultaneously at Tc=TQ=0.06 K. The superconducting transition manifests itself by zero resistance and large diamagnetic susceptibility. The specific heat exhibits a Schottky anomaly peaking at 14 K and magnetization curves measured at 2 K show anisotropic behaviors. The analysis of these data indicates that the crystalline electric field (CEF) ground state of the trivalent Pr ion is the non-Kramers Gamma3 doublet with the quadrupolar degrees of freedom. A sharp peak in the specific heat at 0.06 K has been attributed not to the superconducting transition but to the AFQ transition because the ordering temperature TQ decreases in B || [100] but increases in B || [110] and B || [111] with increasing B up to 6 T. This anisotropic behavior of TQ(B) can be well explained by a two-sublattice mean-field calculation, which corroborates the AFQ ordered state below TQ. The entropy release at TQ is only 10% of Rln2 expected for the Gamma3 doublet, suggesting possible interplay between the quadrupolar degrees of freedom and the superconductivity.Comment: 18 page, 6 figures, accepted for publication in Phys. Rev.

Neutron scattering study of magnetic ordering and excitations in the ternary rare-earth diborocarbide Ce^{11}B_2C_2

Neutron scattering experiments have been performed on the ternary rare-earth diborocarbide Ce$^{11}$B$_2$C$_2$. The powder diffraction experiment confirms formation of a long-range magnetic order at $T_{\rm N} = 7.3$ K, where a sinusoidally modulated structure is realized with the modulation vector ${\bm q} = [0.167(3), 0.167(3), 0.114(3)]$. Inelastic excitation spectra in the paramagnetic phase comprise significantly broad quasielastic and inelastic peaks centered at $\hbar \omega \approx 0, 8$ and 65 meV. Crystalline-electric-field (CEF) analysis satisfactorily reproduces the observed spectra, confirming their CEF origin. The broadness of the quasielastic peak indicates strong spin fluctuations due to coupling between localized $4f$ spins and conduction electrons in the paramagnetic phase. A prominent feature is suppression of the quasielastic fluctuations, and concomitant growth of a sharp inelastic peak in a low energy region below $T_{\rm N}$. This suggests dissociation of the conduction and localized $4f$ electrons on ordering, and contrasts the presently observed incommensurate phase with spin-density-wave order frequently seen in heavy fermion compounds, such as Ce(Ru$_{1-x}$La$_x$)$_2$Si$_2$.Comment: accepted for publication in Phys. Rev.

Itinerant-Electron Magnet of the Pyrochlore Lattice: Indium-Doped YMn2Zn20

We report on a ternary intermetallic compound, "YMn2Zn20", comprising a pyrochlore lattice made of Mn atoms. A series of In-doped single crystals undergo no magnetic long-range order down to 0.4 K, in spite of the fact that the Mn atom carries a local magnetic moment at high temperatures, showing Curie-Weiss magnetism. However, In-rich crystals exhibit spin-glass transitions at approximately 10 K due to a disorder arising from the substitution, while, with decreasing In content, the spin-glass transition temperature is reduced to 1 K. Then, heat capacity divided by temperature approaches a large value of 280 mJ K-2 mol-1, suggesting a significantly large mass enhancement for conduction electrons. This heavy-fermion-like behavior is not induced by the Kondo effect as in ordinary f-electron compounds, but by an alternative mechanism related to the geometrical frustration on the pyrochlore lattice, as in (Y,Sc)Mn2 and LiV2O4, which may allow spin entropy to survive down to low temperatures and to couple with conduction electrons.Comment: 5 pages, 4 figures, J. Phys. Soc. Jpn., in pres

Superconductivity in the Ferroquadrupolar State in the Quadrupolar Kondo Lattice PrTi2_2Al20_{20}

The cubic compound PrTi$_2$Al$_{20}$ is a quadrupolar Kondo lattice system that exhibits quadrupolar ordering due to the non-Kramers $\Gamma_3$ ground doublet and has strong hybridization between $4f$ and conduction electrons. Our study using high-purity single crystal reveals that PrTi$_2$Al$_{20}$ exhibits type-II superconductivity at $T_{\rm c} = 200$ mK in the nonmagnetic ferroquadrupolar state. The superconducting critical temperature and field phase diagram suggests moderately enhanced effective mass of $m^*/m_0 \sim 16$

Effects of Impurities with Singlet-Triplet Configuration on Multiband Superconductors

Roles of multipole degrees of freedom in multiband superconductors are investigated in a case of impurities whose low-lying states consist of singlet ground and triplet excited states, which is related to the experimental fact that the transition temperature $T_{\rm c}$ is increased by Pr substitution for La in LaOs$_4$Sb$_{12}$. The most important contribution to the $T_{\rm c}$ increase comes from the inelastic interband scattering of electrons coupled to quadrupole or octupole moments of impurities. It is found that a magnetic field modifies an effective pairing interaction and the scattering anisotropy appears in the field-orientation dependence of the upper critical field $H_{{\rm c}2}$ in the vicinity of $T_{\rm c}$, although a uniaxial anisotropic field is required for experimental detection. This would be proof that the Pr internal degrees of freedom are relevant to the stability of superconductivity in (La$_{1-x}$Pr$_x$)Os$_4$Sb$_{12}$.Comment: 10 pages, 5 figures, to appear in J. Phys. Soc. Jp

Magnetic Phase Diagrams with Possible Field-induced Antiferroquadrupolar Order in TbB2_2C2_2

Magnetic phase diagrams of a tetragonal antiferromagnet TbB$_2$C$_2$ were clarified by temperature and field dependence of magnetization. It is noticeable that the N{\'e}el temperature in TbB$_2$C$_2$ is anomalously enhanced with magnetic fields, in particular the enhancement reaches 13.5 K for the ${}$ direction at 10 T. The magnetization processes as well as the phase diagrams are well interpreted assuming that there appear field-induced antiferroquadrupolar ordered phases in TbB$_2$C$_2$. The phase diagrams of the AFQ compounds in RB$_2$C$_2$ are systematically understood in terms of the competition with AFQ and AFM interactions.Comment: 4 pages, 4 figures, RevTeX

Kondo Effects and Multipolar Order in the cubic PrTr2Al20 (Tr=Ti, V)

Our single crystal study reveals that PrTr2Al20 (Tr = Ti and V) provides the first examples of a cubic {\Gamma}3 nonmagnetic ground doublet system that shows the Kondo effect including a -ln T dependent resistivity. The {\Gamma}3 quadrupolar moments in PrV2Al20 induce anomalous metallic behavior through hybridization with conduction electrons, such as T^{1/2} dependent resistivity and susceptibility below ~ 20 K down to its ordering temperature T_O = 0.6 K. In PrTi2Al20, however, quadrupoles are well-localized and exhibit an order at T_O = 2.0 K. Stronger Kondo coupling in PrV2Al20 than in PrTi2Al20 suppresses quadrupolar ordering, and instead promotes hybridization between the {\Gamma}3 doublet and conduction electrons, leading to most likely the quadrupolar Kondo effect.Comment: 12 pages, 4 figure

Highly anisotropic strain dependencies in PrIr2_2Zn20_{20}

We report thermal expansion and magnetostriction of the cubic non-Kramers system PrIr$_2$Zn$_{20}$ with a non-magnetic $\varGamma_{3}$ ground state doublet. In previous experiments, antiferroquadrupolar order at \hbox{$T_{\mathrm{Q}}=0.11$\,K} and a Fermi liquid state around $B_{\mathrm{c}}\approx5$\,T for \hbox{$\boldsymbol{B}\parallel[001]$}, indicative of possible ferrohastatic order, were discovered. For magnetic fields \hbox{$\boldsymbol{B}\parallel[001]$}, the low temperature longitudinal and transverse thermal expansion and magnetostriction are highly anisotropic. The resulting volume strain is very small, indicating that the Pr valence remains nearly constant as a function of magnetic field. We conclude that the Fermi liquid state around $B_{\mathrm{c}}$ forms through a very little change in c-f hybridization. This result is in sharp contrast to Ce- and Yb-based Kramers Kondo lattices which show significantly larger volume strains due to the high sensitivity of the Kondo temperature to hydrostatic pressure.Comment: 8 pages, 8 figure

Divergent thermal expansion and Grüneisen ratio in a quadrupolar Kondo metal

We report on the low-temperature thermal expansion and magnetostriction of the single-impurity quadrupolar Kondo candidate Y1−xPrxIr2Zn20. In the dilute limit, we find a quadrupolar strain that possesses a singular dependence on temperature T, ɛu∼H2log(1/T), for a small but finite magnetic field H. Together with the previously reported anomalous specific heat C, this implies a quadrupolar Grüneisen ratio Γu=∂Tɛu/C∼H2/[T2log(1/T)] whose divergence for finite H is consistent with the scenario of a quadrupolar Kondo effect. In addition, we find a singular behavior of the isotropic strain ɛB in zero magnetic field resulting in a divergence of both the volume thermal expansion and the volume Grüneisen parameter. We speculate that this behavior might be also induced by putative Kondo correlations via elastic anharmonicities or static strain disorder