arXiv subjects

Laurence Magaud

Publications and source records attributed to Laurence Magaud.

15 recordsLinked to original sources

arXiv2025

Electronic structure and transport in materials with flat bands: 2D materials and quasicrystals

In this review, we present recent works on materials whose common point is the presence of electronic bands of very low dispersion, called "flat bands", which are due to specific atomic order effects without electron interactions. These states are always indicative of some form of confinement and have consequences on the electronic properties. A first part is devoted to the cases where this confinement is due to the long-range geometry of the defect-free structure. We have thus studied periodic approximant structures of quasiperiodic Penrose and octagonal tilings, and twisted bilayers of graphene (TBG) or transition metal dichalcogenides (TMDs) whose rotation angle between the two layers assumes a special value, called "magic angle". In these materials, the flat bands correspond to electronic states distributed over a very large number of atoms (several hundreds or even thousands of atoms). We have shown that their electronic transport properties cannot be described by usual Bloch-Boltzmann theories, because the interband terms of the velocity operator dominate the intraband terms as far as quantum diffusion is concerned. In the case of TBG, flat bands can induce a magnetic state and other electron-electron correlation effects. The second part focuses on two-dimensional nanomaterials in the presence of local point defects that cause resonant electronic states (vacancies, adsorbed atoms or molecules). We present studies on monolayer graphene, twisted or Bernal bilayer graphene, carbon nanotubes, monolayer and multilayer black phosphorene, and monolayer TMDs. A recent result is the discovery that the selective functionalization of a Bernal bilayer graphene sublattice leads to a metallic or insulating behavior depending on the functionalized sublattice type. This result suggests that functionalization can be a key parameter to control the electronic properties of 2D materials.

cond-mat.mes-hall↗

arXiv2020

How to induce superconductivity in epitaxial graphene $via$ remote proximity effect through an intercalated gold layer

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.

cond-mat.supr-con↗

arXiv2020

Decoupling Molybdenum Disulfide from its Substrate by Cesium Intercalation

Intercalation of alkali atoms within the lamellar transition metal dichalcogenides is a possible route toward a new generation of batteries. It is also a way to induce structural phase transitions authorizing the realization of optical and electrical switches in this class of materials. The process of intercalation has been mostly studied in three-dimensional dichalcogenide films. Here, we address the case of a single-layer of molybdenum disulfide (MoS$_2$), deposited on a gold substrate, and intercalated with cesium (Cs) in ultra-clean conditions (ultrahigh vacuum). We show that intercalation decouples MoS$_2$ from its substrate. We reveal electron transfer from Cs to MoS$_2$, relative changes in the energy of the valence band maxima, and electronic disorder induced by structural disorder in the intercalated Cs layer. Besides, we find an abnormal lattice expansion of MoS$_2$, which we relate to immediate vicinity of Cs. Intercalation is thermally activated, and so is the reverse process of de-intercalation. Our work opens the route to a microscopic understanding of a process of relevance in several possible future technologies, and shows a way to manipulate the properties of two-dimensional dichalcogenides by "under-cover" functionalization.

cond-mat.mtrl-sci↗

arXiv2020

Electronic structure and quantum transport in twisted bilayer graphene with resonant scatterers

Staking layered materials revealed to be a very powerful method to tailor their electronic properties. It has indeed been theoretically and experimentally shown that twisted bilayers of graphene (tBLG) with a rotation angle $θ$, forming Moiré pattern, confine electrons in a tunable way as a function of $θ$. Here, we study electronic structure and transport in tBLG using tight-binding numerical calculations in commensurate twisted bilayer structures and a pertubative continuous theory, which is valid for not too small angles ($θ> \sim 2^\circ $). This two approaches allow to understand the effect of $θ$ on the local density of states, the electron lifetime due to disorder, the dc-conducitivity and the quantum correction of the conductivity due to multiple scattering effects. We distinguished the cases where disorder is equaly distributed in the two layer or only in one layer. When only one layer is disordered, diffusion properties depends strongly on $θ$, showing thus the effect of Moiré electronic localisation at intermediate angles, $\sim 2^\circ < θ< \sim 20^\circ$.

cond-mat.mes-hall↗

arXiv2020

Depressions by stacking faults in nanorippled graphene on metals

A broad variety of defects has been observed in two-dimensional materials. Many of these defects can be created by top-down methods such as electron irradiation or chemical etching, while a few of them are created along bottom-up processes, in particular during the growth of the material, in which case avoiding their formation can be challenging. This occurs e.g. with dislocations, Stone-Wales defects, or atomic vacancies in graphene. Here we address a defect that has been observed repeatedly since 2007 in epitaxial graphene on metal surfaces like Ru(0001) and Re(0001), but whose nature has remained elusive thus far. This defect has the appearance of a vacant hill in the periodically nanorippled topography of graphene, which comes together with a moir{é} pattern. Based on atomistic simulations and scanning tunneling microscopy/spectroscopy measurements, we argue that such defects are topological in nature and that their core is a stacking fault patch, either in graphene, surrounded by loops of non-hexagonal carbon rings, or in the underlying metal. We discuss the possible origin of these defects in relation with recent reports of metastable polycyclic carbon molecules forming upon graphene growth. Like other defects, the vacant hills may be considered as deleterious in the perspective of producing high quality graphene. However, provided they can be organized in graphene, they might allow novel optical, spin, or electronic properties to be engineered.

cond-mat.mtrl-sci↗

arXiv2018

Weakly Trapped, Charged, and Free Excitons in Single-Layer MoS2 in the Presence of Defects, Strain, and Charged Impurities

Few- and single-layer MoS2 host substantial densities of defects. They are thought to influence the doping level, the crystal structure, and the binding of electron-hole pairs. We disentangle the concomitant spectroscopic expression of all three effects and identify to what extent they are intrinsic to the material or extrinsic to it, i.e., related to its local environment. We do so by using different sources of MoS2 -- a natural one and one prepared at high pressure and high temperature -- and different substrates bringing varying amounts of charged impurities and by separating the contributions of internal strain and doping in Raman spectra. Photoluminescence unveils various optically active excitonic complexes. We discover a defect-bound state having a low binding energy of 20 meV that does not appear sensitive to strain and doping, unlike charged excitons. Conversely, the defect does not significantly dope or strain MoS2. Scanning tunneling microscopy and density functional theory simulations point to substitutional atoms, presumably individual nitrogen atoms at the sulfur site. Our work shows the way to a systematic understanding of the effect of external and internal fields on the optical properties of two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2018

Graphene as a Mechanically Active, Deformable Two-Dimensional Surfactant

In crystal growth, surfactants are additive molecules used in dilute amount or as dense, permeable layers to control surface morphologies. Here, we investigate the properties of a strikingly different surfactant: a two-dimensional and covalent layer with close atomic packing, graphene. Using in situ, real time electron microscopy, scanning tunneling microscopy, kinetic Monte Carlo simulations, and continuum mechanics calculations, we reveal why metallic atomic layers can grow in a two-dimensional manner below an impermeable graphene membrane. Upon metal growth, graphene dynamically opens nanochannels called wrinkles, facilitating mass transport, while at the same time storing and releasing elastic energy via lattice distortions. Graphene thus behaves as a mechanically active, deformable surfactant. The wrinkle-driven mass transport of the metallic layer intercalated between graphene and the substrate is observed for two graphene-based systems, characterized by different physico-chemical interactions, between graphene and the substrate, and between the intercalated material and graphene. The deformable surfactant character of graphene that we unveil should then apply to a broad variety of species, opening new avenues for using graphene as a two-dimensional surfactant forcing the growth of flat films, nanostructures and unconventional crystalline phases.

cond-mat.mtrl-sci↗

arXiv2016

Electronic properties of asymmetrically doped twisted graphene bilayers

Rotated graphene bilayers form an exotic class of nanomaterials with fascinating electronic properties governed by the rotation angle theta. For large rotation angles, the electron eigenstates are restricted to one layer and the bilayer behaves like two decoupled graphene layer. At intermediate angles, Dirac cones are preserved but with a lower velocity and van Hove singularities are induced at energies where the two Dirac cones intersect. At very small angles, eigenstates become localized in peculiar moire zones. We analyse here the effect of an asymmetric doping for a series of commensurate rotated bilayers on the basis of tight binding calculations of their band dispersions, density of states, participation ratio and diffusive properties. While a small doping level preserves the theta dependence of the rotated bilayer electronic structure, larger doping induces a further reduction of the band velocity in the same way of to a further reduction of the rotation angle.

cond-mat.mes-hall↗

arXiv2016

Universal classification of twisted, strained and sheared graphene moiré superlattices

Moiré superlattices in graphene supported on various substrates have opened a new avenue to engineer graphene's electronic properties. Yet, the exact crystallographic structure on which their band structure depends remains highly debated. In this scanning tunneling microscopy and density functional theory study, we have analysed graphene samples grown on multilayer graphene prepared onto SiC and on the close-packed surfaces of Re and Ir with ultra-high precision. We resolve small-angle twists and shears in graphene, and identify large unit cells comprising more than 1,000 carbon atoms and exhibiting non-trivial nanopatterns for moiré superlattices, which are commensurate to the graphene lattice. Finally, a general formalism applicable to any hexagonal moiré is presented to classify all reported structures.

cond-mat.mtrl-sci↗

arXiv2014

Convergent Fabrication of a Nanoporous Two-Dimensional Carbon Network from an Aldol Condensation on Metal Surfaces

We report a convergent surface polymerization reaction scheme on Au(111), based on a triple aldol condensation, yielding a carbon-rich, covalent nanoporous two-dimensional network. The reaction is not self-poisoning and proceeds up to a full surface coverage. The deposited precursor molecules 1,3,5-tri(4'-acetylphenyl) first form supramolecular assemblies that are converted to the porous covalent network upon heating. The formation and structure of the network and of the intermediate steps are studied with scanning tunneling microscopy, Raman spectroscopy and density functional theory.

cond-mat.mtrl-sci↗

arXiv2009

Graphene buffer layer on Si-terminated SiC : a multi-minima energy surface studied with an empirical interatomic potential

The atomistic structure of the graphene buffer layer on Si-terminated SiC is studied using a modified environment-dependent interatomic potential (EDIP). The investigation of equilibrium state by conjuguate gradients suffers from a complex multi-minima energy surface. A dedicated procedure is therefore presented to provide a suitable initial configuration on the way to the minimum. The result forms an hexagonal pattern with unsticked rods to release the misfit with the surface. The structure presents an agreement with the global pattern obtained by experiments and even with the details of an ab initio calculation.

cond-mat.mtrl-sci↗

arXiv2009

Localization of Dirac electrons by Moire patterns in graphene bilayers

We study the electronic structure of two Dirac electron gazes coupled by a periodic Hamiltonian such as it appears in rotated graphene bilayers. Ab initio and tight-binding approaches are combined and show that the spatially periodic coupling between the two Dirac electron gazes can renormalize strongly their velocity. We investigate in particular small angles of rotation and show that the velocity tends to zero in this limit. The localization is confirmed by an analysis of the eigenstates which are localized essentially in the AA zones of the Moire patterns.

cond-mat.mes-hall↗

arXiv2008

Few layers graphene on 6H-SiC(000-1): an STM study

We have analyzed by Scanning Tunnelling Microscopy (STM) thin films made of few (3-5) graphene layers grown on the C terminated face of 6H-SiC in order to identify the nature of the azimuthal disorder reported in this material. We observe superstructures which are interpreted as Moiré patterns due to a misorientation angle between consecutive layers. The presence of stacking faults is expected to lead to electronic properties reminiscent of single layer graphene even for multilayer samples. Our results indicate that this apparent electronic decoupling of the layers can show up in STM data.

cond-mat.mtrl-sci↗

arXiv2007

Electron states of mono- and bilayer graphene on SiC probed by STM

We present a scanning tunneling microscopy (STM) study of a gently-graphitized 6H-SiC(0001) surface in ultra high vacuum. From an analysis of atomic scale images, we identify two different kinds of terraces, which we unambiguously attribute to mono- and bilayer graphene capping a C-rich interface. At low temperature, both terraces show $(\sqrt{3}\times \sqrt{3})$ quantum interferences generated by static impurities. Such interferences are a fingerprint of $π$-like states close to the Fermi level. We conclude that the metallic states of the first graphene layer are almost unperturbed by the underlying interface, in agreement with recent photoemission experiments (A. Bostwick et al., Nature Physics 3, 36 (2007))

cond-mat.mtrl-sci↗

arXiv2007

Electronic structure of epitaxial graphene layers on SiC: effect of the substrate

Recent transport measurements on thin graphite films grown on SiC show large coherence lengths and anomalous integer quantum Hall effects expected for isolated graphene sheets. This is the case eventhough the layer-substrate epitaxy of these films implies a strong interface bond that should induce perturbations in the graphene electronic structure. Our DFT calculations confirm this strong substrate-graphite bond in the first adsorbed carbon layer that prevents any graphitic electronic properties for this layer. However, the graphitic nature of the film is recovered by the second and third absorbed layers. This effect is seen in both the (0001)and $(000\bar{1})$ 4H SiC surfaces. We also present evidence of a charge transfer that depends on the interface geometry. It causes the graphene to be doped and gives rise to a gap opening at the Dirac point after 3 carbon layers are deposited in agreement with recent ARPES experiments (T.Ohta et al, Science {\bf 313} (2006) 951).

cond-mat.mtrl-sci↗