Determination of spin Hamiltonian in the Ni4_4 magnetic molecule

Magnetic excitations in a Ni$_4$ magnetic molecule were investigated by inelastic neutron scattering and bulk susceptibility ($\chi_\text{bulk}$) techniques. The magnetic excitation spectrum obtained from the inelastic neutron scattering experiments exhibits three modes at energy transfers of $\hbar\omega=0.5$, 1.35, and 1.6 meV. We show that the energy, momentum, and temperature dependences of the inelastic neutron scattering data and $\chi_\text{bulk}$ can be well reproduced by an effective spin Hamiltonian consisted of intra-molecule exchange interactions, a single-ionic anisotropy, biquadratic interactions, and Zeeman term. Under a hydrostatic pressure, the bulk magnetization decreases with increasing pressure, which along with the biquadratic term indicates spin-lattice coupling present in this system.Comment: 6 pages, 6 figures, and 2 table

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.

Detailed Measurements of Characteristic Profiles of Magnetic Diffuse Scattering in ErB2_2C2_2

Detailed neutron diffraction measurements on a single crystalline ErB$_2$C$_2$ were performed. We observed magnetic diffuse scattering which consists of three components just above the transition temperatures, which is also observed in characteristic antiferroquadrupolar ordering compounds HoB$_2$C$_2$ and TbB$_2$C$_2$. The result of this experiments indicates that the antiferroquadrupolar interaction is not dominantly important as a origin of the magnetic diffuse scattering.Comment: 5 pages, 5 figures, submitted to J. Phys. Soc. Jp

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.

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

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 $m^*/m_0 \sim 16$

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

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