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Register a new userSchottky anomaly and short-range antiferromagnetic correlations in filled skutterudites Pr$_{1-x}$Eu$_x$Pt$_4$Ge$_{12}$
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By performing a series of thermodynamic measurements in an applied magnetic field $H_{textrm{ext}}$, we investigated the effects of Eu substitution on the Pr sites in filled skutterudite compound Pr$_{1-x}$Eu$_x$Pt$_4$Ge$_{12}$ ($ 0 leq x leq 1$). A heat capacity Schottky anomaly is present over the whole doping range. For the samples with $x > 0.5$, these Schottky anomaly peaks shift to lower temperature with increasing $H_{textrm{ext}}$. We argue that this behavior reflects the antiferromagnetic (AFM) ordering of the Eu moments, as the AFM transition is suppressed by $H_{textrm{ext}}$. The Schottky peaks in the samples with $x leq 0.5$ shift to higher temperatures with increasing magnetic field, signaling the presence of an internal magnetic field due to short-range AFM correlations induced by magnetic moments of neighboring Eu sites. In low $H_{textrm{ext}}$, the Schottky gaps show a non-linear relationship with $H_{textrm{ext}}$ as the magnetic moments become weakly magnetized. In high $H_{textrm{ext}}$, the magnetic moments of Eu sites become completely aligned with $H_{textrm{ext}}$. Thus, increasing $H_{textrm{ext}}$ does not further increase the magnetization, hence the Schottky gaps increase linearly with $H_{textrm{ext}}$
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Motivated by current research efforts towards exploring the interplay between magnetism and superconductivity in multiband electronic systems, we have investigated the effects of Eu substitution through thermodynamic measurements on the superconducting filled skutterudite alloys Pr$_{1-x}$Eu$_x$Pt$_4$Ge$_{12}$. An increase in Eu concentration leads to a suppression of the superconducting transition temperature consistent with an increase of magnetic entropy due to Eu local moments. While the low-temperature heat capacity anomaly is present over the whole doping range, we find that in alloys with $xleq0.5$ the Schottky peaks in the heat capacity in the superconducting state appear to be due to Zeeman splitting by an internal magnetic field. Our theoretical modeling suggests that this field is a result of the short-range antiferromagnetic correlations between the europium ions. For the samples with $x > 0.5$, the peaks in the heat capacity signal the onset of antiferromagnetic (AFM) ordering of the Eu moments.
The superconducting state of the filled skutterudite alloy series Pr$_{1-x}$La$_{x}$Pt$_{4}$Ge$_{12}$ has been systematically studied by specific heat, zero-field muon spin relaxation ($mu$SR), and superconducting critical field measurements. An additional inhomogeneous local magnetic field, indicative of broken time-reversal symmetry (TRS), is observed in the superconducting states of the alloys. For $x lesssim 0.5$ the broken-TRS phase sets in below a temperature $T_m$ distinctly lower than the superconducting transition temperature $T_c$. For $x gtrsim 0.5$ $T_m approx T_c$. The local field strength decreases as $x to 1$, where LaPt$_{4}$Ge$_{12}$ is characterized by conventional pairing. The lower critical field $H_{c1}(T)$ of PrPt$_{4}$Ge$_{12}$ shows the onset of a second quadratic temperature region below $T_q sim T_m$. Upper critical field $H_{c2}(T)$ measurements suggest multiband superconductivity, and point gap nodes are consistent with the specific heat data. In Pr$_{1-x}$La$_{x}$Pt$_{4}$Ge$_{12}$ only a single specific heat discontinuity is observed at $T_c$, in contrast to the second jump seen in PrOs$_{4}$Sb$_{12}$ below $T_c$. These results suggest that superconductivity in PrPt$_{4}$Ge$_{12}$ is characterized by a complex order parameter.
Thermal conductivity measurements were performed on single crystal samples of the superconducting filled skutterudite compounds PrOs$_4$Sb$_{12}$ and PrRu$_4$Sb$_{12}$ both as a function of temperature and magnetic field applied perpendicular to the heat current. In zero magnetic field, the low temperature electronic thermal conductivity of PrRu$_4$Sb$_{12}$ is vanishingly small, consistent with a fully-gapped Fermi surface. For PrOs$_4$Sb$_{12}$, however, we find clear evidence for residual electronic conduction as the temperature tends to zero Kelvin which is consistent with the presence of nodes in the superconducting energy gap. The field dependence of the electronic conductivity for both compounds shows a rapid rise immediately above H$_{c1}$ and significant structure over the entire vortex state. In the fully gapped superconductor PrRu$_4$Sb$_{12}$, this is interpreted in terms of multi-band effects. In PrOs$_4$Sb$_{12}$, we consider the Doppler shift of nodal quasiparticles at low fields and multiband effects at higher fields.
The Pr-rich end of the alloy series Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ has been studied using muon spin rotation and relaxation. The end compound PrOs$_4$Sb$_{12}$ is an unconventional heavy-fermion superconductor, which exhibits a spontaneous magnetic field in the superconducting phase associated with broken time-reversal symmetry. No spontaneous field is observed in the Nd-doped alloys for x $>$ 0.05. The superfluid density is insensitive to Nd concentration, and no Nd$^{3+}$ static magnetism is found down to the lowest temperatures of measurement. Together with the slow suppression of the superconducting transition temperature with Nd doping, these results suggest anomalously weak coupling between Nd spins and conduction-band states.
Resistivity measurements were performed on Pr$_{1-x}$La$_x$Os$_4$Sb$_{12}$ single crystals at temperatures down to 20 mK and in fields up to 18 T. The results for dilute-Pr samples ($x=0.3$ and 0.67) are consistent with model calculations performed assuming a singlet crystalline-electric-field (CEF) ground state. The residual resistivity of these crystals features a smeared step centered around 9 T, the predicted crossing field for the lowest CEF levels. The CEF contribution to the magnetoresistance has a weaker-than-calculated dependence on the field direction, suggesting that interactions omitted from the CEF model lead to avoided crossing in the effective levels of the Pr$^{3+}$ ion. The dome-shaped magnetoresistance observed for $x = 0$ and 0.05 cannot be reproduced by the CEF model, and likely results from fluctuations in the field-induced antiferroquadrupolar phase.
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