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Register a new userTuning from Frustrated Magnetism to Superconductivity in Quasi-One-Dimensional KCr$_3$As$_3$ Through Hydrogen Doping
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We report the charge doping of KCr$_3$As$_3$ via H intercalation. We show that the previously reported ethanol bath deintercalation of K$_2$Cr$_3$As$_3$ to KCr$_3$As$_3$ has a secondary effect whereby H from the bath enters the quasi-one-dimensional Cr$_6$As$_6$ chains. Furthermore, we find that - contrary to previous interpretations - the difference between non-superconducting as-grown KCr$_3$As$_3$ samples and superconducting hydrothermally annealed samples is not a change in crystallinity but due to charge doping, with the latter treatment increasing the H concentration in the CrAs tubes effectively electron-doping the 133 compound. These results suggest a new stoichiometry KH$_x$Cr$_3$As$_3$, that superconductivity arises from a suppressed magnetic order via a tunable parameter and pave the way for the first charge-doped phase diagram in these materials.
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Following the discovery of superconductivity in quasi-one-dimensional K$_2$Cr$_3$As$_3$ containing [(Cr$_3$As$_3$)$^{2-}$]$_{infty}$ chains [J. K. Bao et al., arXiv: 1412.0067 (2014)], we succeeded in synthesizing an analogous compound, Rb$_2$Cr$_3$As$_3$, which also crystallizes in a hexagonal lattice. The replacement of K by Rb results in an expansion of $a$ axis by 3%, indicating a weaker interchain coupling in Rb$_2$Cr$_3$As$_3$. Bulk superconductivity emerges at 4.8 K, above which the normal-state resistivity shows a linear temperature dependence up to 35 K. The estimated upper critical field at zero temperature exceeds the Pauli paramagnetic limit by a factor of two. Furthermore, the electronic specific-heat coefficient extrapolated to zero temperature in the mixed state increases with $sqrt{H}$, suggesting existence of nodes in the superconducting energy gap. Hence Rb$_2$Cr$_3$As$_3$ manifests itself as another example of unconventional superconductor in the Cr$_3$As$_3$-chain based system.
We find a lattice instability in the superconductor KCr$_3$As$_3$, corresponding to a distortion of the Cr metallic wires in the crystal structure. This distortion couples strongly to both the electronic and magnetic properties, in particular by making the electronic structure much more nearly one-dimensional, and by shifting the compound away from magnetism. We discuss the implications of these results in the context of the possibly unconventional superconductivity of this phase.
We present neutron total scattering and density functional theory studies on quasi-one-dimensional superconducting K$_2$Cr$_3$As$_3$ revealing a frustrated structural instability. Our first principles calculations find a significant phonon instability which, under energy minimization, corresponds to a frustrated orthorhombic distortion. In diffraction studies we find large and temperature independent atomic displacement parameters which pair distribution analyses confirms and shows as resulting from highly localized orthorhombic distortions of the CrAs sublattice and coupled K displacements. These results suggest a far more complex phase diagram than previously assumed for this unusual superconductor with the likelihood of subtle interplays of structure, electron-phonon and magnetic interactions.
We report the discovery of bulk superconductivity (SC) at 6.1 K in a quasi-one-dimensional (Q1D) chromium pnictide K$_2$Cr$_3$As$_3$ which contains [(Cr$_3$As$_3$)$^{2-}$]$_{infty}$ double-walled subnano-tubes with face-sharing Cr$_{6/2}$ (As$_{6/2}$) octahedron linear chains in the inner (outer) wall. The material has a large electronic specific-heat coefficient of 70$sim$75 mJ K$^{-2}$ mol$^{-1}$, indicating significantly strong electron correlations. Signature of non-Fermi liquid behavior is shown by the linear temperature dependence of resistivity in a broad temperature range from 7 to 300 K. Unconventional SC is preliminarily manifested by the estimated upper critical field exceeding the Pauli limit by a factor of three to four. The title compound represents a rare example that possibly unconventional SC emerges in a Q1D system with strong electron correlations.
I study the lattice dynamics and electron-phonon coupling in non-centrosymmetric quasi-one-dimensional K$_2$Cr$_3$As$_3$ using density functional theory based first principles calculations. The phonon dispersions show stable phonons without any soft-mode behavior. They also exhibit features that point to a strong interaction of K atoms with the lattice. I find that the calculated Eliashberg spectral function shows a large enhancement around 50 cm$^{-1}$. The phonon modes that show large coupling involve in-plane motions of all three species of atoms. The $mathbf{q}$ dependent electron-phonon coupling decreases strongly away from the $q_z = 0$ plane. The total electron-phonon coupling is large with a value of $lambda_{textrm{ep}} = 3.0$, which readily explains the experimentally observed large mass enhancement.
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