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Register a new userEnhanced superconductivity in few-layer TaS$_2$ due to healing by oxygenation
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When approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional materials. Superconductivity is generally thought to be vulnerable to these effects, but here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS$_2$). Our first-principles calculations show that incorporation of oxygen into the TaS$_2$ crystal lattice is energetically favourable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the carrier density to the intrinsic value of TaS$_2$. Strikingly, this leads to a strong enhancement of the electron-phonon coupling, by up to 80% in the highly-oxygenated limit. Using transport measurements on fresh and aged (oxygenated) few-layer TaS$_2$, we found a marked increase of the superconducting critical temperature ($T_{mathrm{c}}$) upon aging, in agreement with our theory, while concurrent electron microscopy and electron-energy loss spectroscopy confirmed the presence of sulfur vacancies in freshly prepared TaS$_2$ and incorporation of oxygen into the crystal lattice with time. Our work thus reveals the mechanism by which certain atomic-scale defects can be beneficial to superconductivity and opens a new route to engineer $T_{mathrm{c}}$ in ultrathin materials.
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The superconducting TMD 4Hb-TaS$_2$ consists of alternating layers of H and T structures, which in their bulk form are metallic and Mott-insulating, respectively. Recently, this compound has been proposed as a candidate chiral superconductor, due to an observed enhancement of the muon spin relaxation at $T_c$. 4Hb-TaS$_2$ also exhibits a puzzling $T$-linear specific heat at low temperatures, which is unlikely to be caused by disorder. Elucidating the origin of this behavior is an essential step in discerning the true nature of the superconducting ground state. Here, we propose a simple model that attributes the $T$-linear specific heat to the emergence of a robust multi-band gapless superconducting state. We show that an extended regime of gapless superconductivity naturally appears when the pair-breaking scattering rate on distinct Fermi-surface pockets differs significantly, and the pairing interaction is predominantly intra-pocket. Using a tight-binding model derived from first-principle calculations, we show that the pair-breaking scattering rate promoted by slow magnetic fluctuations on the T layers, which arise from proximity to a Mott transition, can be significantly different in the various H-layer dominated Fermi pockets depending on their hybridization with T-layer states. Thus, our results suggest that the ground state of 4Hb-TaS$_2$ consists of Fermi pockets displaying gapless superconductivity, which are shunted by superconducting Fermi pockets that are nearly decoupled from the T-layers.
Two-dimensional transition metal dichalcogenides (TMDs) have been attracting significant interest due to a range of properties, such as layer-dependent inversion symmetry, valley-contrasted Berry curvatures, and strong spin-orbit coupling (SOC). Of particular interest is niobium diselenide (NbSe2), whose superconducting state in few-layer samples is profoundly affected by an unusual type of SOC called Ising SOC. Combined with the reduced dimensionality, the latter stabilizes the superconducting state against magnetic fields up to ~35 T and could lead to other exotic properties such as nodal and crystalline topological superconductivity. Here, we report transport measurements of few-layer NbSe$_2$ under in-plane external magnetic fields, revealing an unexpected two-fold rotational symmetry of the superconducting state. In contrast to the three-fold symmetry of the lattice, we observe that the magnetoresistance and critical field exhibit a two-fold oscillation with respect to an applied in-plane magnetic field. We find similar two-fold oscillations deep inside the superconducting state in differential conductance measurements on NbSe$_2$/CrBr$_3$ superconductor-magnet junctions. In both cases, the anisotropy vanishes in the normal state, demonstrating that it is an intrinsic property of the superconducting phase. We attribute the behavior to the mixing between two closely competing pairing instabilities, namely, the conventional s-wave instability typical of bulk NbSe$_2$ and an unconventional d- or p-wave channel that emerges in few-layer NbSe2. Our results thus demonstrate the unconventional character of the pairing interaction in a few-layer TMD, opening a new avenue to search for exotic superconductivity in this family of 2D materials.
In a Kondo lattice system, suppression of effective Kondo coupling leads to the breakdown of the heavy-electron metal and a change in the electronic structure. Spin triplet superconductivity in the Kondo lattice UTe2 appears to be associated with spin fluctuations originating from incipient ferromagnetic order. Here we show clear evidence of twofold enhancement of spin-triplet superconductivity near the pressure-driven suppression of the Kondo coherence, implying that superconductivity is strengthened by the affiliated growth of both spin and charge fluctuations. The coherent Kondo state discontinuously transitions to ferromagnetic order at higher pressures. Application of magnetic field tunes the system back across a first-order phase boundary. Straddling this phase boundary, we find another example of reentrant superconductivity in UTe2. In addition to spin fluctuations associated with ferromagnetism, our results show that a Kondo-driven Fermi surface instability may be playing a role in stabilizing spin triplet superconductivity.
Layered van der Waals (vdW) materials are emerging as one of the most versatile directions in the field of quantum condensed matter physics. They allow an unprecedented control of electronic properties via stacking of different types of two-dimensional (2D) materials. A fascinating frontier, largely unexplored, is the stacking of strongly-correlated phases of matter in vdW materials. Here, we study 4Hb-TaS$_2$, which naturally realizes an alternating stacking of a Mott insulator, recently reported as a gapless spin-liquid candidate(1T-TaS$_2$), and a 2D superconductor (1H-TaS$_2$). This raises the question of how these two components affect each other. We find a superconducting ground state with a transition temperature of 2.7K, which is significantly elevated compared to the 2H polytype (Tc=0.7K). Strikingly, the superconducting state exhibits signatures of time-reversal-symmetry breaking abruptly appearing at the superconducting transition, which can be naturally explained by a chiral superconducting state.
Bound quasiparticles, negatively charged trions and neutral excitons, are associated with the direct optical transitions at the K-points of the Brillouin zone for monolayer MoS$_2$. The change in the carrier concentration, surrounding dielectric constant and defect concentration can modulate the photoluminescence and Raman spectra. Here we show that exposing the monolayer MoS$_2$ in air to a modest laser intensity for a brief period of time enhances simultaneously the photoluminescence (PL) intensity associated with both trions and excitons, together with $sim$ 3 to 5 times increase of the Raman intensity of first and second order modes. The simultaneous increase of PL from trions and excitons cannot be understood based only on known-scenario of depletion of electron concentration in MoS$_2$ by adsorption of O$_2$ and H$_2$O molecules. This is explained by laser induced healing of defect states resulting in reduction of non-radiative Auger processes. This laser healing is corroborated by an observed increase of intensity of both the first order and second order 2LA(M) Raman modes by a factor of $sim$ 3 to 5. The A$_{1g}$ mode hardens by $sim$ 1.4 cm$^{-1}$ whereas the E$^1_{2g}$ mode softens by $sim$ 1 cm$^{-1}$. The second order 2LA(M) Raman mode at $sim$ 440 cm$^{-1}$ shows an increase in wavenumber by $sim$ 8 cm$^{-1}$ with laser exposure. These changes are a combined effect of change in electron concentrations and oxygen-induced lattice displacements.
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