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Ambient Pressure Structural Quantum Critical Point in the Phase Diagram of (Ca$_x$Sr$_{1-x}$)$_3$Rh$_4$Sn$_{13}$

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 Added by Swee K. Goh
 Publication date 2014
  fields Physics
and research's language is English




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The quasi-skutterudite superconductor Sr$_3$Rh$_4$Sn$_{13}$ features a pronounced anomaly in electrical resistivity at $T^*sim$138 K. We show that the anomaly is caused by a second-order structural transition, which can be tuned to 0 K by applying physical pressure and chemical pressure via the substitution of Ca for Sr. A broad superconducting dome is centred around the structural quantum critical point. Detailed analysis of the tuning parameter dependence of $T^*$ as well as insights from lattice dynamics calculations strongly support the existence of a structural quantum critical point at ambient pressure when the fraction of Ca is 0.9 (i.e., $x_c=0.9$). This establishes (Ca$_x$Sr$_{1-x}$)$_3$Rh$_4$Sn$_{13}$ series as an important system for exploring the physics of structural quantum criticality without the need of applying high pressures.



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We perform optical spectroscopy measurement across the charge density wave (CDW) phase transitions on single-crystal samples of Sr$_{3}$Rh$_{4}$Sn$_{13}$ and (Sr$_{0.5}$Ca$_{0.5}$)$_{3}$Rh$_{4}$Sn$_{13}$. Formation of CDW energy gap was clearly observed for both single-crystal samples when they undergo the phase transitions. The existence of a Drude component in $sigma_1(omega)$ below TCDW indicates that the Fermi surface is only partially gapped in the CDW state. The obtained value of 2$Delta$/K$_{B}$T$_{CDW}$ is roughly 13 for both Sr$_{3}$Rh$_{4}$Sn$_{13}$ and (Sr$_{0.5}$Ca$_{0.5}$)$_{3}$Rh$_{4}$Sn$_{13}$ compounds. The value is considerably larger than the mean-field value based on the weak-coupling BCS theory. The observed spectral feature in (Sr$_{x}$Ca$_{1-x}$)$_{3}$Rh$_{4}$Sn$_{13}$ resembles those seen in many other CDW systems.
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The comprehensive research of the electronic structure, thermodynamic and electrical transport properties reveals the existence of inhomogeneous superconductivity due to structural disorder in Ca$_3$Rh$_4$Sn$_{13}$ doped with La (Ca$_{3-x}$La$_x$Rh$_4$Sn$_{13}$) or Ce (Ca$_{3-x}$Ce$_x$Rh$_4$Sn$_{13}$) with superconducting critical temperatures $T_c^{star}$ higher than those ($T_c$) observed in the parent compounds. The $T-x$ diagrams and the entropy $S(x)_T$ isotherms well document the relation between degree of an atomic disorder and separation of the {it high-temperature} $T_c^{star}$ and $T_c$-bulk phases. In these dirty superconductors with the mean free path much smaller than the coherence length, the Werthamer-Helfand-Hohenber theoretical model does not well fits the $H_{c2}(T)$ data. We suggest that this can result from two-band superconductivity or from the presence of strong inhomogeneity in these systems. The multiband model very well describes the $H-T$ dependencies, but the present results as well as our previous studies give arguments for the scenario based on the presence of nanoscopic inhomogeneity of the superconducting state. We also revisited the nature of structural phase transition at $T^{star}sim 130-170$ K and documented that there might be another precursor transition at higher temperatures. The impact of the magnetic Ce-Ce correlations on the increase of $T_c$ in respect to the critical temperatures of Ca$_{3-x}$La$_x$Rh$_4$Sn$_{13}$ is also discussed.
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