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Register a new userSignature of Unconventional Superconductivity in a Copper-based Metal-Organic Framework with Perfect Kagome Structure
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Recently, the superconductivity in a metal-organic framework (MOF) has been discovered for the first time in copper(II) benzenehexathiolate ([Cu$_3$(C$_6$S$_6$)]$_n$, Cu-BHT). The Cu atoms form a two-dimensional perfect Kagome lattice, which has the potential to host a metallic quantum spin liquid state. Here we present high-precision measurements of in-plane magnetic penetration depth $lambda$ in Cu-BHT films down to 40,mK. The temperature dependence of $lambda$ shows a non-exponential, quasi-linear behavior at low temperatures, suggesting that unconventional superconductivity with low-energy quasiparticle excitations is realized in this system. With the reported non-Fermi liquid behavior, this finding implies that MOFs can provide a flexible platform to investigate the superconducting pairing mechanisms in the presence of spin frustration and strong quantum fluctuations.
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Metal-organic frameworks (MOFs), which are self-assemblies of metal ions and organic ligands, provide a tunable platform to search a new state of matter. A two-dimensional (2D) perfect kagome lattice, whose geometrical frustration is a key to realizing quantum spin liquids, has been formed in the ${pi}$-${d}$ conjugated 2D MOF [Cu$_{3}$(C$_{6}$S$_{6}$)]$_{n}$ (Cu-BHT). The recent discovery of its superconductivity with a critical temperature $T_{rm c}$ of 0.25,kelvin raises fundamental questions about the nature of electron pairing. Here, we show that Cu-BHT is a strongly correlated unconventional superconductor with extremely low superfluid density. A nonexponential temperature dependence of superfluid density is observed, indicating the possible presence of superconducting gap nodes. The magnitude of superfluid density is much smaller than those in conventional superconductors, and follows the Uemuras relation of strongly correlated superconductors. These results imply that the unconventional superconductivity in Cu-BHT originates from electron correlations related to spin fluctuations of kagome lattice.
The recently discovered family of vanadium-based kagome metals with topological band structures offer a new opportunity to study frustrated, correlated and topological quantum states. These layered compounds are nonmagnetic and undergo charge density wave (CDW) transitions before developing superconductivity at low temperatures. Here we report the observation of unconventional superconductivity and pair density wave (PDW) in the vanadium-based kagome lattice CsV3Sb5 using scanning tunneling microscope/spectroscopy (STM/STS) and Josephson STS. The differential conductance exhibits a V-shaped pairing gap about 0.5 meV below a transition temperature Tc about 2.3 K. Superconducting phase coherence is observed by Josephson effect and Cooper-pair tunneling to a superconducting tip. We find that CsV3Sb5 is a strong-coupling superconductor (2delta/kBTc about 5) and coexists with 4a0 unidirectional and 2x2 charge order. Remarkably, we discover a 4a0/3 bidirectional PDW accompanied by spatial modulations of the coherence peak and gap-depth in the tunneling conductance. We term the latter as a roton-PDW that can produce a commensurate vortex-antivortex lattice to account for the observed conductance modulations. Above Tc, we observe long-range ordered 4a0 unidirectional and 2a0 bidirectional CDW and a large V-shaped pseudogap in the density of state. Electron-phonon calculations attribute the 2x2 CDW to phonon softening induced structural reconstruction, but the phonon mediated pairing cannot describe the observed strong-coupling superconductor. Our findings show that electron correlations in the charge sector can drive the 4a0 unidirectional CDW, unconventional superconductivity, and roton-PDW with striking analogies to the phenomenology of cuprate high-Tc superconductors, and provide the groundwork for understanding their microscopic origins in the vanadium-based kagome superconductors.
The mechanism of superconductivity in cuprates remains one of the big challenges of condensed matter physics.High Tc cuprates crystallize into layered perovskite structure featuring copper oxygen octahedral coordination. Due to the Jahn Teller effect in combination with the strong static Coulomb interaction, the octahedra in high Tc cuprates are elongated along the c axis, leading to a 3dx2-y2 orbital at the top of the band structure wherein the doped holes reside.This scenario gives rise to two dimensional characteristics in high Tc cuprates that favor d wave pairing symmetry. Here we report superconductivity in a cuprate Ba2CuO4-y wherein the local octahedron is in a very exceptional compressed version.The Ba2CuO4-y compound was synthesized at high pressure at high temperatures, and shows bulk superconductivity with critical temperature Tc above 70 K at ambient conditions. This superconducting transition temperature is more than 30 K higher than the Tc for the isostructural counterparts based on classical La2CuO4. X-ray absorption measurements indicate the heavily doped nature of the Ba2CuO4-y superconductor. In compressed octahedron the 3d3z2-r2 orbital will be lifted above the 3dx2-y2 orbital, leading to significant three dimensional nature in addition to the conventional 3dx2-y2 orbital. This work sheds important new light on advancing our comprehensive understanding of the superconducting mechanism of high Tc in cuprate materials.
Recently superconductivity was discovered in the Kagome metal AV3Sb5 (A = K, Rb, and Cs), which has an ideal Kagome lattice of vanadium. These V-based superconductors also host charge density wave (CDW) and topological nontrivial band structure. Here we report the ultralow-temperature thermal conductivity and high pressure resistance measurements on CsV3Sb5 with Tc = 2.5 K, the highest among AV3Sb5. A finite residual linear term of thermal conductivity at zero magnetic field and its rapid increase in fields suggest nodal superconductivity. By applying pressure, the Tc of CsV3Sb5 increases first, then decreases to lower than 0.3 K at 11.4 GPa, showing a clear first superconducting dome peaked around 0.8 GPa. Above 11.4 GPa, superconductivity re-emerges, suggesting a second superconducting dome. Both nodal superconductivity and superconducting domes point to unconventional superconductivity in this V-based superconductor. While our finding of nodal superconductivity puts a strong constrain on the pairing state of the first dome, which should be related to the CDW instability, the superconductivity of the second dome may present another exotic pairing state in this ideal Kagome lattice of vanadium.
Understanding the competition between superconductivity and other ordered states (such as antiferromagnetic or charge-density-wave (CDW) state) is a central issue in condensed matter physics. The recently discovered layered kagome metal AV3Sb5 (A = K, Rb, and Cs) provides us a new playground to study the interplay of superconductivity and CDW state by involving nontrivial topology of band structures. Here, we conduct high-pressure electrical transport and magnetic susceptibility measurements to study CsV3Sb5 with the highest Tc of 2.7 K in AV3Sb5 family. While the CDW transition is monotonically suppressed by pressure, superconductivity is enhanced with increasing pressure up to P1~0.7 GPa, then an unexpected suppression on superconductivity happens until pressure around 1.1 GPa, after that, Tc is enhanced with increasing pressure again. The CDW is completely suppressed at a critical pressure P2~2 GPa together with a maximum Tc of about 8 K. In contrast to a common dome-like behavior, the pressure-dependent Tc shows an unexpected double-peak behavior. The unusual suppression of Tc at P1 is concomitant with the rapidly damping of quantum oscillations, sudden enhancement of the residual resistivity and rapid decrease of magnetoresistance. Our discoveries indicate an unusual competition between superconductivity and CDW state in pressurized kagome lattice.
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