The role of hyperfine coupling in magnetic and quadrupolar ordering of Pr3Pd20Si6

We study the ternary clathrate Pr3Pd20Si6 in specific heat and AC-susceptibility measurements on a high-quality single crystal, distinguishing antiferromagnetic (AFM) and antiferroquadrupolar (AFQ) ordering on two sublattices of inequivalent Pr sites. The specific heat shows the direct involvement of nuclear spin degrees of freedom in the AFM ordering, which is well supported by our calculation of the hyperfine level scheme without adjustable parameters. Pr3Pd20Si6 is therefore one of the rare materials where the nuclear moments are involved in the formation of the magnetic ground state.Comment: 5 pages, 5 figure

Magnetic-Field-Independent Ultrasonic Dispersions in the Magnetically Robust Heavy Fermion System SmOs4Sb12

Elastic properties of the filled skutterudite compound SmOs$_4$Sb$_{12}$ have been investigated by ultrasonic measurements. The elastic constant $C_{11}(\omega)$ shows two ultrasonic dispersions at $\sim$15 K and $\sim$53 K for frequencies $\omega$ between 33 and 316 MHz, which follow a Debye-type formula with Arrhenius-type temperature-dependent relaxation times, and remain unchanged even with applied magnetic fields up to 10 T. The corresponding activation energies were estimated to be $E_2$ = 105 K and $E_1$ = 409 K, respectively. The latter, $E_1$, is the highest value reported so far in the Sb-based filled skutterudites. The presence of magnetically robust ultrasonic dispersions in SmOs$_4$Sb$_{12}$ implies a possibility that an emergence of a magnetically insensitive heavy fermion state in this system is associated with a novel local charge degree of freedom which causes the ultrasonic dispersion.Comment: 5 pages, 4 figure

Tunneling and rattling in clathrate crystal

We present tunneling and rattling motions of an off-center guest atom in cage referring to a clathrate crystal La_3Pd_{20}Ge_6. The elastic constant C_{44} of La_3Pd_{20}Ge_6 shows a Debye-type dispersion around 20 K obeying a relaxation time tau = tau_0exp(E/k_{B}T) with an attempt time tau_0 = 2.0*10^{-12} sec and an activation energy E = 197 K. At low temperatures below 3 K down to 20 mK, the C_{44} shows a softening of C_{44} = C_{44}^0(T-T_C^0)/(T-Theta) with T_C^0 = -337.970 mK and Theta = -338.044 mK. These facts are attributed to two different types of the off-center motions with Gamma_5 symmetry in 4a-site cage of La_3Pd_{20}Ge_6, a thermally activated rattling motion over the potential hill and a tunneling motion through the potential hill at low temperatures.Comment: 5 pages, 4 figures, to be published Phys. Rev.

Quadrupolar effect and rattling motion in heavy fermion superconductor PrOs_4Sb_{12}

The elastic properties of a filled skutterudite PrOs_4Sb_{12} with a heavy Fermion superconductivity at T_C=1.85 K have been investigated. The elastic softening of (C_{11}-C_{12})/2 and C_{44} with lowering temperature down to T_C indicates that the quadrupolar fluctuation due to the CEF state plays a role for the Cooper paring in superconducting phase of PrOs_4Sb_{12}. A Debye-type dispersion in the elastic constants around 30 K revealed a thermally activated Gamma_{23} rattling due to the off-center Pr-atom motion obeying tau=tau_{0}exp(E/k_{B}T) with an attempt time tau_0=8.8*10^{-11} sec and an activation energy E=168 K. It is remarkable that the charge fluctuation of the off-center motion with Gamma_{23} symmetry may mix with the quadrupolar fluctuation and enhance the elastic softening of (C_{11}-C_{12})/2 just above T_C.Comment: 5 pages, 4 figures, to be published to Phys. Rev.

Ferroquadrupole ordering and Gamma_5 rattling motion in clathrate compound Ce_3Pd_20Ge_6

Lattice effects in a cerium based clathrate compound Ce_3Pd_20Ge_6 with a cubic Cr_23C_6-type structure have been investigated by ultrasonic and thermal expansion measurements. Elastic softenings of (C_11-C_12)/2 and C_44 proportional to the reciprocal temperature 1/T above T_Q1 = 1.25 K are well described in terms of the quadrupole susceptibility for the ground state Gamma_8 quartet. A huge softening of 50 % in (C_11-C_12)/2 and a spontaneous expansion DL/L = 1.9x10^-4 along the [001] direction in particular indicate the ferroquadrupole ordering of O_2^0 below T_Q1. The elastic anomalies associated with the antiferromagnetic ordering at T_N2 = 0.75 K and the incommensurate antiferromagnetic ordering are also found. Notable frequency dependence of C_44 around 10 K is accounted for by the Debye-type dispersion indicating a Gamma_5 rattling motion of an off-center Ce ion along the [111] direction with eight fractionally occupied positions around the 4a site in a cage. The thermally activated Gamma_5 rattling motion obeying a relaxation time t = t_0exp(E/k_BT) with an attempt time t_0 = 3.1x10^-11 sec and an activation energy E = 70 K dies out with decreasing temperature, and then the off-center tunneling state of Ce ion in the 4a-site cage will appear at low temperatures.Comment: 11 pages, 15 figures, to be published on Phys. Rev.

Γ3-type Lattice Instability and the Hidden Order of URu2Si2

We have performed ultrasonic measurements on single-crystalline URu2Si2 with pulsed magnetic fields, in order to check for possible lattice instabilities due to the hybridized state and the hidden-order state of this compound. The elastic constant (C11-C12)/2, which is associated with a response to the Γ3-type symmetry-breaking (orthorhombic) strain field, shows a three-step increase at H 35 T for H k c at low temperatures, where successive meta-magnetic transitions are observed in the magnetization. We discovered a new fact that the absolute change of the softening of (C11-C12)/2 in the temperature dependence is quantitatively recovered at the suppression of hybridized-electronic state and the hidden order in high-magnetic field for H k c associated with the successive transitions. The present results suggest that the Γ3-type lattice instability, is related to both the emergence of the hybridized electronic state and the hidden-order parameter of URu2Si2. On the other hand, magnetic fields H k [100] and [110] enhance the softening of (C11-C12)/2 in the hidden order phase, while no step-like anomaly is observed up to 68.7 T.We discuss the limitation of the localized-electron picture for describing these features of URu2Si2 by examination of a crystalline electric field model in terms of mean-field theory