Thermoelectric properties of Ba-Cu-Si clathrates

Thermoelectric properties of the type-I clathrates Ba$_8$Cu$_x$Si$_{46-x}$ ($3.6 \leq x \leq 7$, $x$ = nominal Cu content) are investigated both experimentally and theoretically. The polycrystalline samples are prepared either by melting, ball milling and hot pressing or by melt spinning, hand milling and hot pressing techniques. Temperature-dependent electrical resistivity, $\rho(T)$, and the Seebeck coefficient, $S(T)$, measurements reveal metal-like behavior for all samples. For $x = 5$ and 6, density functional theory calculations are performed for deriving the enthalpy of formation and the electronic structure which is exploited for the calculation of Seebeck coefficients and conductivity within Boltzmann's transport theory. For simulating the properties of doped clathrates the rigid band model is applied. On the basis of the density functional theory results the experimentally observed compositional dependence of $\rho(T)$ and $S(T)$ of the whole sample series is analyzed. The highest dimensionless thermoelectric figure of merit $ZT$ of 0.28 is reached for a melt-spun sample at $600^{\circ}$C. The relatively low $ZT$ values in this system are attributed to the too high charge carrier concentrations.Comment: 11 pages, 13 figures, submitted to Phys. Rev.

Unconventional superconductivity in weakly correlated, non-centrosymmetric Mo3Al2C\rm{Mo_3Al_2C}

Electrical resistivity, specific heat and NMR measurements classify non-centrosymmetric $\rm Mo_3Al_2C$ ($\beta$-Mn type, space group $P4_132$) as a strong-coupled superconductor with $T_c = 9$~K deviating notably from BCS-like behaviour. The absence of a Hebbel-Slichter peak, a power law behaviour of the spin-lattice relaxation rate (from $^{27}$Al NMR), a $T^3$ temperature dependence of the specific heat and a pressure enhanced $T_c$ suggest unconventional superconductivity with a nodal structure of the superconducting gap. Relativistic DFT calculations reveal a splitting of degenerate electronic bands due to the asymmetric spin-orbit coupling, favouring a mix of spin-singlet and spin triplet components in the superconducting condensate, in absence of strong correlations among electrons.Comment: 4 pages, 5 figure

Intermediate valence behavior in CeCo9Si4

The novel ternary compound CeCo$_9$Si$_4$ has been studied by means of specific heat, magnetisation, and transport measurements. Single crystal X-ray Rietveld refinements reveal a fully ordered distribution of Ce, Co and Si atoms with the tetragonal space group I4/mcm isostructural with other RCo9Si4. The smaller lattice constants of CeCo9Si4 in comparison with the trend established by other RCo9Si4 is indicative for intermediate valence of cerium. While RCo9Si4 with R= Pr, .. Tb, and Y show ferromagnetism and LaCo9Si4 is nearly ferromagnetic, CeCo9Si4 remains paramagnetic even in external fields as large as 40 T, though its electronic specific heat coefficient (g~190 mJ/molK^2) is of similar magnitude as that of metamagnetic LaCo9Si4 and weakly ferromagnetic YCo9Si4.Comment: 2 pages, 3 figures, submitted to SCES 0

Superconductivity in novel Ge-based skutterudites: {Sr,Ba}Pt_4Ge_{12}

Combining experiments and ab initio models we report on $\rm SrPt_4Ge_{12}$ and $\rm BaPt_4Ge_{12}$ as members of a novel class of superconducting skutterudites, where Sr or Ba atoms stabilize a framework entirely formed by Ge-atoms. Below $T_c=5.35$ K, and 5.10 K for $\rm BaPt_4Ge_{12}$ and $\rm SrPt_4Ge_{12}$, respectively, electron-phonon coupled superconductivity emerges, ascribed to intrinsic features of the Pt-Ge framework, where Ge-$p$ states dominate the electronic structure at the Fermi energy.Comment: 4 pages, 4 figures, accepted for publication in PR

Heavy fermion superconductivity and magnetic order in non-centrosymmetric CePt3SiCePt_3Si

$\rm CePt_3Si$ is a novel heavy fermion superconductor, crystallising in the $\rm CePt_3B$ structure as a tetragonally distorted low symmetry variant of the $\rm AuCu_3$ structure type. $\rm CePt_3Si$ exhibits antiferromagnetic order at $T_N \approx 2.2$ K and enters into a heavy fermion superconducting state at $T_c \approx 0.75$ K. Large values of $H_{c2}' \approx -8.5$ T/K and $H_{c2}(0) \approx 5$ T refer to heavy quasiparticles forming Cooper pairs. Hitherto, $\rm CePt_3Si$ is the first heavy fermion superconductor without a center of symmetry.Comment: 4 pages, 4 figure

Terahertz superlattice parametric oscillator

We report a GaAs/AlAs superlattice parametric oscillator. It was pumped by a microwave field (power few mW) and produced 3rd harmonic radiation (frequency near 300 GHz). The nonlinearity of the active superlattice was due to Bragg reflections of conduction electrons at the superlattice planes. A theory of the nonlinearity indicates that parametric oscillation should be possible up to frequencies above 10 THz. The active superlattice may be the object of further studies of predicted extraordinary nonlinearities for THz fields.Comment: 10 pages, 4 figure

Heavy Fermion Behavior, Crystalline Electric Field Effects, and Weak Ferromagnetism in SmOs_{4}Sb_{12}

The filled skutterudite compound SmOs_{4}Sb_{12} was prepared in single crystal form and characterized. The SmOs_{4}Sb_{12} crystals have the LaFe_{4}P_{12}-type structure with lattice parameter a = 9.3085 Angstroms. Specific heat measurements indicate a large electronic specific heat coefficient of ~880 mJ/mol K^{2}, from which an enhanced effective mass m^{*} ~ 170 m_{e} is estimated. The specific heat data also suggest crystalline electric field (CEF) splitting of the Sm^{3+} J = 5/2 multiplet into a Gamma_{7} doublet ground state and a Gamma_{8} quartet excited state separated by 37 K. Electrical resistivity rho(T) measurements reveal a decrease in rho(T) below ~50 K that is consistent with CEF splitting of ~33 K between a Gamma_(7) doublet ground state and Gamma_{8} quartet excited state. Specific heat and magnetic susceptibility measurements display a possible weak ferromagnetic transition at ~2.6 K, which could be an intrinsic property of SmOs_4Sb_{12} or possibly due to an unknown impurity phase.Comment: 24 pages, 11 Postscript figures, to be published in Physical Review

A new polymorphic material? Structural degeneracy of ZrMn_2

Based on density functional calculations, we propose that ZrMn_2 is a polymorphic material. We predict that at low temperatures the cubic C15, and the hexagonal C14 and C36 structures of the Laves phase compound ZrMn_2 are nearly equally stable within 0.3 kJmol^{-1} or 30 K. This degeneracy occurs when the Mn atoms magnetize spontaneously in a ferromagnetic arrangement forming the states of lowest energy. From the temperature dependent free energies at T approx 160K we predict a transition from the most stable C15 to the C14 structure, which is the experimentally observed structure at elevated temperatures.Comment: 4 pages, 3 figure

Itinerant electron metamagnetism in LaCo9_9Si4_4

The strongly exchange enhanced Pauli paramagnet LaCo$_9$Si$_4$ is found to exhibit an itinerant metamagnetic phase transition with indications for metamagnetic quantum criticality. Our investigation comprises magnetic, specific heat, and NMR measurements as well as ab-initio electronic structure calculations. The critical field is about 3.5 T for $H||c$ and 6 T for $H\bot c$, which is the lowest value ever found for rare earth intermetallic compounds. In the ferromagnetic state there appears a moment of about 0.2 $\mu_B$/Co at the $16k$ Co-sites, but sigificantly smaller moments at the 4d and $16l$ Co-sites.Comment: 11 pages, 5 figures, PRB Rapid Communication, in prin