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Register a new userElectronic structure and phonon instabilities in the vicinity of the structural transition and superconductivity of (Sr,Ca)$_3$Ir$_4$Sn$_{13}$
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David A. Tompsett
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The nature of the lattice instability connected to the structural transition and superconductivity of (Sr,Ca)$_3$Ir$_4$Sn$_{13}$ is not yet fully understood. In this work density functional theory (DFT) calculations of the phonon instabilities as a function of chemical and hydrostatic pressure show that the primary lattice instabilities in Sr$_3$Ir$_4$Sn$_{13}$ lie at phonon modes of wavevectors $mathbf{q}=(0.5,0,0)$ and $mathbf{q}=(0.5,0.5,0)$. Following these modes by calculating the energy of supercells incorporating the mode distortion results in an energy advantage of -14.1 meV and -9.0 meV per formula unit respectively. However, the application of chemical pressure to form Ca$_3$Ir$_4$Sn$_{13}$ reduces the energetic advantage of these instabilities, which is completely removed by the application of a hydrostatic pressure of 35 kbar to Ca$_3$Ir$_4$Sn$_{13}$. The evolution of these lattice instabilities is consistent with experimental phase diagram. The structural distortion associated with the mode at $mathbf{q}=(0.5,0.5,0)$ produces a distorted cell with the same space group symmetry as the experimentally refined low temperature structure. Furthermore, calculation of the deformation potential due to these modes quantitatively demonstrates a strong electron-phonon coupling. Therefore, these modes are likely to be implicated in the structural transition and superconductivity of this system.
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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.
In a superconductor that lacks inversion symmetry, the spatial part of the Cooper pair wave function has a reduced symmetry, allowing for the mixing of spin-singlet and spin-triplet Cooper pairing channels and thus providing a pathway to a non-trivial superconducting state. Materials with a non-centrosymmetric crystal structure and with strong spin-orbit coupling are a platform to realize these possibilities. Here, we report the synthesis and characterisation of high quality crystals of Sn$_4$As$_3$, with non-centrosymmetric unit cell ($R3m$). We have characterised the normal and superconducting state using a range of methods. Angle-resolved photoemission spectroscopy shows a multiband Fermi surface and the presence of two surface states, confirmed by Density-functional theory calculations. Specific heat measurements reveal a superconducting critical temperature of $T_csim 1.14$ K and an upper critical magnetic field of $H_cgtrsim 7$ mT, which are both confirmed by ultra-low temperature scanning tunneling microscopy and spectroscopy. Scanning tunneling spectroscopy shows a fully formed superconducting gap, consistent with conventional $s$-wave superconductivity.
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.
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.
We measured the pressure dependence of in-plane resistivity $rho_{ab}$ in the recently-discovered iron-based superconductor Ca$_{10}$(Ir$_{4}$As$_{8}$)(Fe$_{2-x}$Ir$_{x}$As$_{2}$)$_{5}$, which shows a unique structural phase transition in the absence of magnetic ordering, with a superconducting transition temperature $T_{rm c}$ = 16 K and structural phase transition temperature $T_{rm s}$ $simeq$ 100 K at ambient pressure. $T_{rm c}$ and $T_{rm s}$ are suppressed on applying pressure and disappear at approximately 0.5 GPa, suggesting a relationship between superconductivity and structure. Ca$_{10}$(Ir$_{4}$As$_{8}$)(Fe$_{2-x}$Ir$_{x}$As$_{2}$)$_{5}$ is a rather rare example in which the superconductivity appears only in a low-temperature ordered phase. The fact that the change in the crystal structure is directly linked with superconductivity suggests that the crystal structure as well as magnetism are important factors governing superconductivity in iron pnictides.
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