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.

Observation of Modulated Quadrupolar Structures in PrPb3

Neutron diffraction measurements have been performed on the cubic compound PrPb3 in a [001] magnetic field to examine the quadrupolar ordering. Antiferromagnetic components with q=(1/2+-d 1/2 0), (1/2 1/2+-d 0) (d~1/8) are observed below the transition temperature TQ (0.4 K at H=0) whose amplitudes vary linear with H and vanish at zero field, providing the first evidence for a modulated quadrupolar phase. For H<1 T, a non-square modulated state persists even below 100 mK suggesting quadrupole moments associated with a Gamma3 doublet ground state to be partially quenched by hybridization with conduction electrons.Comment: Physical Review Letters, in press. 4 pages, 4 figure

Neutron scattering study on spin correlations and fluctuations in the transition-metal-based magnetic quasicrystal Zn-Fe-Sc

Spin correlations and fluctuations in the 3d-transition-metal-based icosahedral quasicrystal Zn-Fe-Sc have been investigated by neutron scattering using polycrystalline samples. Magnetic diffuse scattering has been observed in the elastic experiment at low temperatures, indicating development of static short-range-spin correlations. In addition, the inelastic scattering experiment detects a $Q$-independent quasielastic signal ascribed to single-site relaxational spin fluctuations. Above the macroscopic freezing temperature $T_{\rm f} \simeq 7$ K, the spin relaxation rate shows Arrhenius-type behavior, indicating thermally activated relaxation process. In contrast, the relaxation rate remains finite even at the lowest temperature, suggesting a certain quantum origin for the spin fluctuations below $T_{\rm f}$.Comment: To be published 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 $m^*/m_0 \sim 16$

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

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