arXiv subjects

Johann Coraux

Publications and source records attributed to Johann Coraux.

At least 37 records · Page 2Linked to original sources

arXiv2020

Structure of graphene and a surface carbide grown on the (0001) surface of rhenium

Transition metal surfaces catalyse a broad range of thermally-activated reactions involving carbon-containing-species -- from atomic carbon to small hydrocarbons or organic molecules, and polymers. These reactions yield well-separated phases, for instance graphene and the metal surface, or, on the contrary, alloyed phases, such as metal carbides. Here, we investigate carbon phases on a rhenium (0001) surface, where the former kind of phase can transform into the latter. We find that this transformation occurs with increasing annealing time, which is hence not suitable to increase the quality of graphene. Our scanning tunneling spectroscopy and reflection high-energy electron diffraction analysis reveal that repeated short annealing cycles are best suited to increase the lateral extension of the structurally coherent graphene domains. Using the same techniques and with the support of density functional theory calculations, we next unveil, in real space, the symmetry of the many variants (two six-fold families) of a rhenium surface carbide observed with diffraction since the 1970s, and finally propose models of the atomic details. One of these models, which nicely matches the microscopy observations, consists of parallel rows of eight aligned carbon trimers with a so-called $(7\times\sqrt{\mathrm{19}})$ unit cell with respect to Re(0001).

cond-mat.mtrl-sci↗

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

Anharmonicity in Raman-active phonon modes in atomically thin MoS$_2$

Phonon-phonon anharmonic effects have a strong influence on the phonon spectrum; most prominent manifestation of these effects are the softening (shift in frequency) and broadening (change in FWHM) of the phonon modes at finite temperature. Using Raman spectroscopy, we studied the temperature dependence of the FWHM and Raman shift of $\mathrm{E_{2g}^1}$ and $\mathrm{A_{1g}}$ modes for single-layer and natural bilayer MoS$_2$ over a broad range of temperatures ($8 < $T$ < 300$ K). Both the Raman shift and FWHM of these modes show linear temperature dependence for $T>100$ K, whereas they become independent of temperature for $T<100$ K. Using first-principles calculations, we show that three-phonon anharmonic effects intrinsic to the material can account for the observed temperature-dependence of the line-width of both the modes. It also plays an important role in determining the temperature-dependence of the frequency of the Raman modes. The observed evolution of the line-width of the A$_{1g}$ mode suggests that electron-phonon processes are additionally involved. From the analysis of the temperature-dependent Raman spectra of MoS$_2$ on two different substrates -- SiO$_2$ and hexagonal boron nitride, we disentangle the contributions of external stress and internal impurities to these phonon-related processes. We find that the renormalization of the phonon mode frequencies on different substrates is governed by strain and intrinsic doping. Our work establishes the role of intrinsic phonon anharmonic effects in deciding the Raman shift in MoS$_2$ irrespective of substrate and layer number.

cond-mat.mes-hall↗

arXiv2020

In-plane magnetic domains and Néel-like domain walls in thin flakes of the room temperature CrTe$_2$ van der Waals ferromagnet

The recent discovery of magnetic van der Waals materials has triggered a wealth of investigations in materials science, and now offers genuinely new prospects for both fundamental and applied research. Although the catalogue of van der Waals ferromagnets is rapidly expanding, most of them have a Curie temperature below 300 K, a notable disadvantage for potential applications. Combining element-selective x-ray magnetic imaging and magnetic force microscopy, we resolve at room temperature the magnetic domains and domains walls in micron-sized flakes of the CrTe$_2$ van der Waals ferromagnet. Flux-closure magnetic patterns suggesting in-plane six-fold symmetry are observed. Upon annealing the material above its Curie point (315 K), the magnetic domains disappear. By cooling back down the sample, a different magnetic domain distribution is obtained, indicating material stability and lack of magnetic memory upon thermal cycling. The domain walls presumably have Néel texture, are preferentially oriented along directions separated by 120 degrees, and have a width of several tens of nanometers. Besides microscopic mapping of magnetic domains and domain walls, the coercivity of the material is found to be of a few mT only, showing that the CrTe$_2$ compound is magnetically soft. The coercivity is found to increase as the volume of the material decreases.

cond-mat.mtrl-sci↗

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

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↗

arXiv2019

Room temperature 2D ferromagnetism in few-layered 1$T$-CrTe$_{2}$

Spin-related electronics using two dimensional (2D) van der Waals (vdW) materials as a platform are believed to hold great promise for revolutionizing the next generation spintronics. Although many emerging new phenomena have been unravelled in 2D electronic systems with spin long-range orderings, the scarcely reported room temperature magnetic vdW material has thus far hindered the related applications. Here, we show that intrinsic ferromagnetically aligned spin polarization can hold up to 316 K in a metallic phase of 1$T$-CrTe$_{2}$ in the few-layer limit. This room temperature 2D long range spin interaction may be beneficial from an itinerant enhancement. Spin transport measurements indicate an in-plane room temperature negative anisotropic magnetoresistance (AMR) in few-layered CrTe$_{2}$, but a sign change in the AMR at lower temperature, with -0.6$\%$ at 300 K and +5$\%$ at 10 K, respectively. This behavior may originate from the specific spin polarized band structure of CrTe$_{2}$. Our findings provide insights into magnetism in few-layered CrTe$_{2}$, suggesting potential for future room temperature spintronic applications of such 2D vdW magnets.

cond-mat.mes-hall↗

arXiv2019

Confined step-flow growth of Cu intercalated between graphene and a Ru(0001) surface

By comparing the growth of Cu thin films on bare and graphene-covered Ru(0001) surfaces, we demonstrate the role of graphene as a surfactant allowing the formation of flat Cu films. Low-energy electron microscopy, X-ray photoemission electron microscopy and X-ray absorption spectroscopy reveal that depositing Cu at 580 K leads to distinct behaviors on both types of surfaces. On bare Ru, a Stranski-Krastanov growth is observed, with first the formation of an atomically flat and monolayer-thick wetting layer, followed by the nucleation of three-dimensional islands. In sharp contrast, when Cu is deposited on a graphene-covered Ru surface under the very same conditions, Cu intercalates below graphene and grows in a step-flow manner: atomically-high growth fronts of intercalated Cu form at the graphene edges, and extend towards the center of the flakes. Our findings suggest potential routes in metal heteroepitaxy for the control of thin film morphology.

cond-mat.mtrl-sci↗

arXiv2018

Coherence and density dynamics of excitons in a single-layer MoS$_2$ reaching the homogeneous limit

We measure the coherent nonlinear response of excitons in a single-layer of molybdenum disulphide embedded in hexagonal boron nitride, forming a $h$-BN/MoS$_2$/$h$-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton homogeneous and inhomogeneous broadenings. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultra-fast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the $h$-BN and imperfections in the encapsulation process.

cond-mat.mes-hall↗

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↗

arXiv2017

Intercalating cobalt between graphene and iridium (111): a spatially-dependent kinetics from the edges

Using low-energy electron microscopy, we image in real time the intercalation of a cobalt monolayer between graphene and the (111) surface of iridium. Our measurements reveal that the edges of a graphene flake represent an energy barrier to intercalation. Based on a simple description of the growth kinetics, we estimate this energy barrier and find small, but substantial, local variations. These local variations suggest a possible influence of the graphene orientation with respect to its substrate and of the graphene edge termination on the energy value of the barrier height. Besides, our measurements show that intercalated cobalt is energetically more favorable than cobalt on bare iridium, indicating a surfactant role of graphene.

cond-mat.mtrl-sci↗

arXiv2017

High-Yield Proximity-Induced Chemical Vapor Deposition of Graphene Over Millimeter-Sized Hexagonal Boron Nitride

We present a transfer-free preparation method for graphene on hexagonal boron nitride (h-BN) crystals by chemical vapor deposition of graphene via a catalytic proximity effect, i.e. activated by a Cu catalyst close-by . We demonstrate the full coverage by monolayer graphene of half-millimeter-sized hexagonal boron nitride crystals exfoliated on a copper foil prior to growth. We demonstrate that the proximity of the copper catalyst ensures high yield with the growth rate estimated between of 2μm/min to 5μm/min . Optical and electron microscopies together with confocal micro-Raman mapping confirm that graphene covers the top surface of h-BN crystals that we attribute to be a lateral growth from the supporting catalytic copper substrate. Structural and electron transport characterization of the in-situ grown graphene present an electronic mobility of about 20, 000cm2/(V.s). Comparison with graphene/h-BN stacks obtained by manual transferring of similar CVD graphene onto h-BN, confirms the better neutrality reached by the self-assembled structures.

cond-mat.mtrl-sci↗

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↗

arXiv2015

Degenerate epitaxy-driven defects in monolayer silicon oxide onto ruthenium

The structure of the ultimately-thin crystalline allotrope of silicon oxide, prepared onto a ruthenium surface, is unveiled down to atomic scale with chemical sensitivity, thanks to high resolution scanning tunneling microscopy and first principle calculations. An ordered oxygen lattice is imaged which coexists with the two-dimensional monolayer oxide. This coexistence signals a displacive transformation from an oxygen reconstructed-Ru(0001) to silicon oxide, along which latterally-shifted domains form, each with equivalent and degenerate epitaxial relationships with the substrate. The unavoidable character of defects at boundaries between these domains appeals for the development of alternative methods capable of producing single-crystalline two-dimensional oxides.

cond-mat.mtrl-sci↗

arXiv2015

Anatomy and giant enhancement of the perpendicular magnetic anisotropy of cobalt-graphene heterostructures

We report strongly enhanced perpendicular magnetic anisotropy (PMA) of Co films by graphene coating from both first-principles and experiments. Our calculations show that graphene can dramatically boost the surface anisotropy of Co films up to twice the value of its pristine counterpart and can extend the out-of-plane effective anisotropy up to unprecedented thickness of 25~Å. These findings are supported by our experiments on graphene coating on Co films grown on Ir substrate. Furthermore, we report layer-resolved and orbital-hybridization-resolved anisotropy analysis which help understanding the physical mechanisms of PMA and more practically can help design structures with giant PMA. As an example, we propose super-exchange stabilized Co-graphene heterostructures with a robust out-of-plane constant effective PMA and linearly increasing interfacial anisotropy as a function of film thickness. These findings point towards possibilities to engineer graphene/ferromagnetic metal heterostructures with giant magnetic anisotropy more than 20 times larger compared to conventional multilayers, which constitutes a hallmark for future graphene and traditional spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2015

Topography of the graphene/Ir(111) moir{é} studied by surface x-ray diffraction

The structure of a graphene monolayer on Ir(111) has been investigated {\it in situ} in the growth chamber by surface x-ray diffraction including the specular rod, which allows disentangling the effect of the sample roughness from that of the nanorippling of graphene and iridium along the moir{é}-like pattern between graphene and Ir(111). Accordingly we are able to provide precise estimates of the undulation associated with this nanorippling, which is small in this weakly interacting graphene/metal system and thus proved difficult to assess in the past. The nanoripplings of graphene and iridium are found in phase, i.e. the in-plane position of their height maxima coincide, but the amplitude of the height modulation is much larger for graphene ($0.379 \pm 0.044$ Å) than, {\it e.g.}, for the topmost Ir layer ($0.017 \pm 0.002$ Å). The average graphene-Ir distance is found to be $3.38 \pm 0.04$ Å.

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↗