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Short-range antiferromagnetic correlations in the superconducting state of filled skutterudite alloys Pr$_{1-x}$Eu$_x$Pt$_4$Ge$_{12}$

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 Added by Ram Adhikari
 Publication date 2018
  fields Physics
and research's language is English




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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.

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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 $H_{textrm{ext}}$
264 - T. Namiki , Y. Aoki , H. Sato 2007
We report on systematic study of superconducting characteristics and Pr crystalline-electric-field (CEF) levels of filled-skutterudite pra ($T_{rm c}$ = 2.33 K). The temperature dependences of the upper critical field $H_{rm c2}$ and the Ginzburg-Landau (Maki) parameter $kappa_2$ suggest an s-wave clean-limit superconductivity. The electronic specific heat coefficient $gamma sim 95$ mJ/K$^2$mol, being $sim 1.5$ times larger than that for lra, indicates $4f$-originating quasiparticle mass enhancement. Magnetic susceptibility $chi(T)$ indicates that the CEF ground state is a $Gamma_1$ singlet and a $Gamma_4^{(1)}$ triplet first excited state lies at $Delta_{rm CEF}sim 30$ K above. Systematic comparison among pos, prs, pra and La-based reference compounds suggests that inelastic exchange- and aspherical-charge-scatterings of conduction electrons from CEF-split $4f$ levels play an essential role for the quasiparticle mass enhancement and the value of $T_{rm c}$ in the Pr-based filled skutterudites.
Superconductivity, magnetic order, and quadrupolar order have been investigated in the filled skutterudite system Pr$_{1-x}$Nd$_{x}$Os$_4$Sb$_{12}$ as a function of composition $x$ in magnetic fields up to 9 tesla and at temperatures between 50 mK and 10 K. Electrical resistivity measurements indicate that the high field ordered phase (HFOP), which has been identified with antiferroquadruoplar order, persists to $x$ $sim$ 0.5. The superconducting critical temperature $T_c$ of PrOs$_4$Sb$_{12}$ is depressed linearly with Nd concentration to $x$ $sim$ 0.55, whereas the Curie temperature $T_{FM}$ of NdOs$_4$Sb$_{12}$ is depressed linearly with Pr composition to ($1-x$) $sim$ 0.45. In the superconducting region, the upper critical field $H_{c2}(x,0)$ is depressed quadratically with $x$ in the range 0 $<$ $x$ $lesssim$ 0.3, exhibits a kink at $x$ $approx$ 0.3, and then decreases linearly with $x$ in the range 0.3 $lesssim$ $x$ $lesssim$ 0.6. The behavior of $H_{c2}(x,0)$ appears to be due to pair breaking caused by the applied magnetic field and the exhange field associated with the polarization of the Nd magnetic moments, in the superconducting state. From magnetic susceptibility measurements, the correlations between the Nd moments in the superconducting state appear to change from ferromagnetic in the range 0.3 $lesssim$ $x$ $lesssim$ 0.6 to antiferromagnetic in the range 0 $<$ $x$ $lesssim$ 0.3. Specific heat measurements on a sample with $x$ $=$ 0.45 indicate that magnetic order occurs in the superconducting state, as is also inferred from the depression of $H_{c2}(x,0)$ with $x$.
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.
Studies of superconductivity in multiband correlated electronic systems has become one of the central topics in condensed matter/materials physics. In this paper, we present the results of thermodynamic measurements on the superconducting filled skutterudite system Pr$_{1-x}$Ce$_x$Pt$_4$Ge$_{12}$ ($ 0 leq x leq 0.2$) to investigate how substitution of Ce at Pr sites affects superconductivity. We find that an increase in Ce concentration leads to a suppression of the superconducting transition temperature from $T_{c}sim 7.9$ K for $x=0$ to $T_csim 0.6$ K for $x=0.14$. Our analysis of the specific heat data for $xleq 0.07$ reveals that superconductivity must develop in at least two bands: the superconducting order parameter has nodes on one Fermi pocket and remains fully gapped on the other. Both the nodal and nodeless gap values decrease, with the nodal gap being suppressed more strongly, with Ce substitution. Ultimately, the higher Ce concentration samples ($x>0.07$) display a nodeless gap only.
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