ABSTRACT: Despite graphene's long list of exceptional electronic properties and many theoretical predictions regarding the possibility of superconductivity in graphene, its direct and unambiguous experimental observation has not been achieved. We searched for superconductivity in weakly interacting, metal decorated graphene crystals assembled into so-called graphene laminates, consisting of well separated and electronically decoupled graphene crystallites. We report robust superconductivity in all Ca-doped graphene laminates. They become superconducting at temperatures (Tc) between ?4 and ?6 K, with Tc's strongly dependent on the confinement of the Ca layer and the induced charge carrier concentration in graphene. We find that Ca is the only dopant that induces superconductivity in graphene laminates above 1.8 K among several dopants used in our experiments, such as potassium, caesium and lithium. By revealing the tunability of the superconducting response through doping and confinement of the metal layer, our work shows that achieving superconductivity in free-standing, metal decorated monolayer graphene is conditional on an optimum confinement of the metal layer and sufficient doping, thereby bringing its experimental realization within grasp.
Project description:There is a great deal of fundamental and practical interest in the possibility of inducing superconductivity in a monolayer of graphene. But while bulk graphite can be made to superconduct when certain metal atoms are intercalated between its graphene sheets, the same has not been achieved in a single layer. Moreover, there is a considerable debate about the precise mechanism of superconductivity in intercalated graphite. Here we report angle-resolved photoelectron spectroscopy measurements of the superconducting graphite intercalation compound CaC6 that distinctly resolve both its intercalant-derived interlayer band and its graphene-derived ?* band. Our results indicate the opening of a superconducting gap in the ?* band and reveal a substantial contribution to the total electron-phonon-coupling strength from the ?*-interlayer interband interaction. Combined with theoretical predictions, these results provide a complete account for the superconducting mechanism in graphite intercalation compounds and lend support to the idea of realizing superconducting graphene by creating an adatom superlattice.
Project description:FeSe layer-based superconductors exhibit exotic and distinctive properties. The undoped FeSe shows nematicity and superconductivity, while the heavily electron-doped KxFe2-ySe2 and single-layer FeSe/SrTiO3 possess high superconducting transition temperatures that pose theoretical challenges. However, a comprehensive study on the doping dependence of an FeSe layer-based superconductor is still lacking due to the lack of a clean means of doping control. Through angle-resolved photoemission spectroscopy studies on K-dosed thick FeSe films and FeSe0.93S0.07 bulk crystals, here we reveal the internal connections between these two types of FeSe-based superconductors, and obtain superconductivity below ? 46?K in an FeSe layer under electron doping without interfacial effects. Moreover, we discover an exotic phase diagram of FeSe with electron doping, including a nematic phase, a superconducting dome, a correlation-driven insulating phase and a metallic phase. Such an anomalous phase diagram unveils the remarkable complexity, and highlights the importance of correlations in FeSe layer-based superconductors.
Project description:Atomically thin films of layered materials such as molybdenum disulfide (MoS2) are of growing interest for the study of phase transitions in two-dimensions through electrostatic doping. Electrostatic doping techniques giving access to high carrier densities are needed to achieve such phase transitions. Here we develop a method of electrostatic doping which allows us to reach a maximum n-doping density of 4 × 10(14)?cm(-2) in few-layer MoS2 on glass substrates. With increasing carrier density we first induce an insulator to metal transition and subsequently an incomplete metal to superconductor transition in MoS2 with critical temperature ?10?K. Contrary to earlier reports, after the onset of superconductivity, the superconducting transition temperature does not depend on the carrier density. Our doping method and the results we obtain in MoS2 for samples as thin as bilayers indicates the potential of this approach.
Project description:The exploitation of interface effects turned out to be a powerful tool for generating exciting material properties. Such properties include magnetism, electronic and ionic transport and even superconductivity. Here, instead of using conventional homogeneous doping to enhance the hole concentration in lanthanum cuprate and achieve superconductivity, we replace single LaO planes with SrO dopant planes using atomic-layer-by-layer molecular beam epitaxy (two-dimensional doping). Electron spectroscopy and microscopy, conductivity measurements and zinc tomography reveal such negatively charged interfaces to induce layer-dependent superconductivity (Tc up to 35?K) in the space-charge zone at the side of the planes facing the substrate, where the strontium (Sr) profile is abrupt. Owing to the growth conditions, the other side exhibits instead a Sr redistribution resulting in superconductivity due to conventional doping. The present study represents a successful example of two-dimensional doping of superconducting oxide systems and demonstrates its power in this field.
Project description:Research on black phosphorus has been experiencing a renaissance over the last years, after the demonstration that few-layer crystals exhibit high carrier mobility and a thickness-dependent bandgap. Black phosphorus is also known to be a superconductor under high pressure exceeding 10?GPa. The superconductivity is due to a structural transformation into another allotrope and accompanied by a semiconductor-metal transition. No superconductivity could be achieved for black phosphorus in its normal orthorhombic form, despite several reported attempts. Here we describe its intercalation by several alkali metals (Li, K, Rb and Cs) and alkali-earth Ca. All the intercalated compounds are found to be superconducting, exhibiting the same (within experimental accuracy) critical temperature of 3.8±0.1?K and practically identical characteristics in the superconducting state. Such universal superconductivity, independent of the chemical composition, is highly unusual. We attribute it to intrinsic superconductivity of heavily doped individual phosphorene layers, while the intercalated layers of metal atoms play mostly a role of charge reservoirs.
Project description:Monolayer graphene exhibits many spectacular electronic properties, with superconductivity being arguably the most notable exception. It was theoretically proposed that superconductivity might be induced by enhancing the electron-phonon coupling through the decoration of graphene with an alkali adatom superlattice [Profeta G, Calandra M, Mauri F (2012) Nat Phys 8(2):131-134]. Although experiments have shown an adatom-induced enhancement of the electron-phonon coupling, superconductivity has never been observed. Using angle-resolved photoemission spectroscopy (ARPES), we show that lithium deposited on graphene at low temperature strongly modifies the phonon density of states, leading to an enhancement of the electron-phonon coupling of up to ? ? 0.58. On part of the graphene-derived ?*-band Fermi surface, we then observe the opening of a ? ? 0.9-meV temperature-dependent pairing gap. This result suggests for the first time, to our knowledge, that Li-decorated monolayer graphene is indeed superconducting, with Tc ? 5.9 K.
Project description:Co-doping of lanthanum and phosphorus in CaFe₂As₂ induces superconductivity at 45 K. This superconducting transition temperature is higher than the 38 K transition in Ba₁-xKxFe₂As₂, which is the maximum found thus far among the 122 phases. Superconductivity with a substantial shielding volume fraction was observed at 0.12 ≤ x ≤ 0.18 and y = 0.06 in Ca₁-xLaxFe₂(As₁-yPy)₂. The superconducting phase of the present system seems to be not adjacent to an antiferromagnetic phase.
Project description:Several research groups have reported on the observation of superconductivity in bilayer graphene structures where single atomic layers of graphene are stacked and then twisted at angles ? forming Moiré superlattices. The characterization of the superconducting state in these 2D materials is an ongoing task. Here we investigate the pairing symmetry of bilayer graphene Moiré superlattices twisted at ??=?1.05°, 1.10° and 1.16° for carrier doping states varied in the range of n?=?(0.5?-?1.5)?·?10<sup>12</sup>?cm<sup>-2</sup> (where superconductivity can be realized) by analyzing the temperature dependence of the upper critical field B<sub>c2</sub>(T) and the self-field critical current J<sub>c</sub>(sf,T) within currently available models - all of which start from phonon-mediated BCS theory - for single- and two-band s-, d-, p- and d?+?id-wave gap symmetries. Extracted superconducting parameters show that only s-wave and a specific kind of p-wave symmetries are likely to be dominant in bilayer graphene Moiré superlattices. More experimental data is required to distinguish between the s- and remaining p-wave symmetries as well as the suspected two-band superconductivity in these 2D superlattices.
Project description:Graphene decorated with 5d transitional metal atoms is predicted to exhibit many intriguing properties; for example iridium adatoms are proposed to induce a substantial topological gap in graphene. We extensively investigated the conductivity of single-layer graphene decorated with iridium deposited in ultra-high vacuum at low temperature (7 K) as a function of Ir concentration, carrier density, temperature, and annealing conditions. Our results are consistent with the formation of Ir clusters of ~100 atoms at low temperature, with each cluster donating a single electronic charge to graphene. Annealing graphene increases the cluster size, reducing the doping and increasing the mobility. We do not observe any sign of an energy gap induced by spin-orbit coupling, possibly due to the clustering of Ir.
Project description:Ever since the discovery of high-Tc superconductivity in layered cuprates, the roles that individual layers play have been debated, due to difficulty in layer-by-layer characterization. While there is similar challenge in many Fe-based layered superconductors, the newly-discovered Ca10(Pt4As8)(Fe2As2)5 provides opportunities to explore superconductivity layer by layer, because it contains both superconducting building blocks (Fe2As2 layers) and intermediate Pt4As8 layers. Cleaving a single crystal under ultra-high vacuum results in multiple terminations: an ordered Pt4As8 layer, two reconstructed Ca layers on the top of a Pt4As8 layer, and disordered Ca layer on the top of Fe2As2 layer. The electronic properties of individual layers are studied using scanning tunneling microscopy/spectroscopy (STM/S), which reveals different spectra for each surface. Remarkably superconducting coherence peaks are seen only on the ordered Ca/Pt4As8 layer. Our results indicate that an ordered structure with proper charge balance is required in order to preserve superconductivity.