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Register a new userTailoring Superconductivity in Large-Area Single-Layer NbSe2 via Self-Assembled Molecular Adlayers
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Added by
Francesco Calavalle
Publication date
2020
fields
Physics
and research's language is
English
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Two-dimensional transition metal dichalcogenides (TMDs) represent an ideal testbench for the search of materials by design, because their optoelectronic properties can be manipulated through surface engineering and molecular functionalization. However, the impact of molecules on intrinsic physical properties of TMDs, such as superconductivity, remains largely unexplored. In this work, the critical temperature (TC) of large-area NbSe2 monolayers is manipulated, employing ultrathin molecular adlayers. Spectroscopic evidence indicates that aligned molecular dipoles within the self-assembled layers act as a fixed gate terminal, collectively generating a macroscopic electrostatic field on NbSe2. This results in an sim 55% increase and a 70% decrease in TC depending on the electric field polarity, which is controlled via molecular selection. The reported functionalization, which improves the air stability of NbSe2, is efficient, practical, up-scalable, and suited to functionalize large-area TMDs. Our results indicate the potential of hybrid 2D materials as a novel platform for tunable superconductivity.
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In certain unconventional superconductors with sizable electronic correlations, the availability of closely competing pairing channels leads to characteristic soft collective fluctuations of the order parameters, which leave fingerprints in many observables and allow to scrutinize the phase competition. Superconducting layered materials, where electron-electron interactions are enhanced with decreasing thickness, are promising candidates to display these correlation effects. For example, while bulk NbSe2 is essentially a conventional superconductor, recent experiments in the thin-film regime have shown evidence of competing unconventional nematic pairing. In this work, we report the existence of a soft collective mode in single-layer NbSe2, observed as a characteristic resonance excitation in high resolution tunneling spectra. This resonance is observed along with higher harmonics, its frequency is anticorrelated with the local superconducting gap, and its amplitude gradually vanishes by increasing the temperature and upon applying a magnetic field up to the critical values (TC and HC2), which sets an unambiguous link to the superconducting state. Aided by a microscopic model, we interpret this resonance as a collective Leggett mode that represents the fluctuation towards a proximate f-wave triplet state, due to subleading attraction in the triplet channel. Our findings demonstrate the fundamental role of correlations in superconducting 2D transition metal dichalcogenides, opening a path towards unconventional superconductivity in simple, scalable and transferable 2D superconductors.
The origin of high-Tc superconductivity remains an enigma even though tremendous research effort and progress have been made on cuprate and iron pnictide superconductors. Aiming to mimic the cuprate-like electronic configuration of transition metal, superconductivity has been recently found in nickelates. This discovery hallmarks a new era in the search and understanding of the high-Tc superconductivity. However, unlike the cuprate and iron pnictide, in which the superconductivity was initially found in a compound containing La, the superconductivity in the nickelate has only been observed in Nd- and Pr-based compounds. This raises a central question of whether the f electron of the rare-earth element is critical for superconductivity in the nickelates. Here, we report the observation of superconductivity in infinite-layer Ca-doped LaNiO2 (La1-xCaxNiO2) thin films and construct their phase diagram. Unlike the metal-insulator transition in Nd- and Pr-based nickelates, the undoped and underdoped La1-xCaxNiO2 thin films are entirely insulating from 300 down to 2 K. A superconducting dome is observed from 0.15<x<0.3 with weakly insulating behavior at the overdoped regime. Moreover, the sign of the Hall coefficient RH changes at low temperature for samples with a higher doping level. However, distinct from the Nd- and Pr-based nickelates, the RH-sign-change temperature remains around 35 K as the doping increases, suggesting a different multiband structure in the La1-xCaxNiO2. These results also emphasize the significant role of lattice correlation on the multiband structures of the infinite-layer nickelates.
This mini review focuses on conductance measurements through molecular junctions containing few tens of molecules, which are fabricated along two approaches: (i) conducting atomic force microscope contacting a self-assembled monolayers on metal surface, and (ii) tiny molecular junctions made of metal nanodot (diameter < 10 nm), covered by fewer than 100 molecules and contacted by a conducting atomic force microscope. In particular, this latter approach has allowed to obtain new results or to revisit previous ones, which are reviewed here: (i) how the electron transport properties of molecular junctions are modified by mechanical constraint, (ii) the role of intermolecular interactions on the shape of conductance histograms of molecular junctions, and (iii) the demonstration that a molecular diode can operate in the microwave regime up to 18 GHz.
Graphene holds promises for exploring exotic superconductivity with Dirac-like fermions. Making graphene a superconductor at large scales is however a long-lasting challenge. A possible solution relies on epitaxially-grown graphene, using a superconducting substrate. Such substrates are scarce, and usually destroy the Dirac character of the electronic band structure. Using electron diffraction (reflection high-energy, and low-energy), scanning tunneling microscopy and spectroscopy, atomic force microscopy, angle-resolved photoemission spectroscopy, Raman spectroscopy, and density functional theory calculations, we introduce a strategy to induce superconductivity in epitaxial graphene $via$ a remote proximity effect, from the rhenium substrate through an intercalated gold layer. Weak graphene-Au interaction, contrasting with the strong undesired graphene-Re interaction, is demonstrated by a reduced graphene corrugation, an increased distance between graphene and the underlying metal, a linear electronic dispersion and a characteristic vibrational signature, both latter features revealing also a slight $p$ doping of graphene. We also reveal that the main shortcoming of the intercalation approach to proximity superconductivity is the creation of a high density of point defects in graphene (10$^{14}$~cm$^{-2}$). Finally, we demonstrate remote proximity superconductivity in graphene/Au/Re(0001), at low temperature.
We propose nanoscale magnetometry via isolated single-spin qubits as a probe of superconductivity in two-dimensional materials. We characterize the magnetic field noise at the qubit location, arising from current and spin fluctuations in the sample and leading to measurable polarization decay of the qubit. We show that the noise due to transverse current fluctuations studied as a function of temperature and sample-probe distance can be used to extract useful information about the transition to a superconducting phase and the pairing symmetry of the superconductor. Surprisingly, at low temperatures, the dominant contribution to the magnetic noise arises from longitudinal current fluctuations and can be used to probe collective modes such as monolayer plasmons and bilayer Josephson plasmons. We also characterize the noise due to spin fluctuations, which allows probing the spin structure of the pairing wave function. Our results provide a non-invasive route to probe the rich physics of two-dimensional superconductors.
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