Superconductivity and crystalline electric field effects in the filled skutterudite series Pr(Os$_{1-x}$Ru$_x$)$_4$Sb$_{12}$

Abstract

X-ray powder diffraction, magnetic susceptibility $\chi(T)$, and electrical resistivity $\rho(T)$ measurements were made on single crystals of the filled skutterudite series Pr(Os$_{1-x}$Ru$_x$)$_4$Sb$_{12}$. One end of the series ($x = 0$) is a heavy fermion superconductor with a superconducting critical temperature $T_{c} = 1.85$ K, while the other end ($x = 1$) is a conventional superconductor with $T_{c} \approx 1$ K. The lattice constant $a$ decreases approximately linearly with increasing Ru concentration $x$. As Ru (Os) is substituted for Os (Ru), $T_{c}$ decreases nearly linearly with substituent concentration and exhibits a minimum with a value of $T_{c} = 0.75$ K at $x = 0.6$, suggesting that the two types of superconductivity compete with one another. Crystalline electric field (CEF) effects in $\chi_\mathrm{dc}(T)$ and $\rho(T)$ due to the splitting of the Pr$^{3+}$ nine-fold degenerate Hund's rule $J = 4$ multiplet are observed throughout the series, with the splitting between the ground state and the first excited state increasing monotonically as $x$ increases. The fits to the $\chi_\mathrm{dc}(T)$ and $\rho(T)$ data are consistent with a $\Gamma_{3}$ doublet ground state for all values of x, although reasonable fits can be obtained for a $\Gamma_{1}$ ground state for $x$ values near the end member compounds ($x = 0$ or $x = 1$).