We report on the structural and transport properties of the smallest dislocation loop in graphene, known as a flower defect. First, by means of advanced experimental imaging techniques, we deduce how flower defects are formed during recrystallization of chemical vapor deposited graphene. We propose that the flower defects arise from a bulge type mechanism in which the flower domains are the grains left over by dynamic recrystallisation. Next, in order to evaluate the use of such defects as possible building blocks for all-graphene electronics, we combine multiscale modeling tools to investigate the structure and the electron and phonon transport properties of large monolayer graphene samples with a random distribution of flower defects. For large enough flower densities, we find that electron transport is strongly suppressed while, surprisingly, hole transport remains almost unaffected. These results suggest possible applications of flowered graphene for electron energy filtering. For the same defect densities, phonon transport is reduced by orders of magnitude as elastic scattering by defects becomes dominant. Heat transport by flexural phonons, key in graphene, is largely suppressed even for very low concentrations.
By limiting the carbon segregation at the copper surface defects, a pulsed chemical vapor deposition method for single layer graphene growth is shown to inhibit the formation of few-layer regions, leading to a fully single-layered graphene homogeneous at the centimeter scale. Graphene field-effect devices obtained after transfer of pulsed grown graphene on oxidized silicon exhibit mobilities above 5000 cm^2.V^-1.s^-1.
Growth of epitaxial graphene on the C-face of SiC has been investigated. Using a confinement controlled sublimation (CCS) method, we have achieved well controlled growth and been able to observe propagation of uniform monolayer graphene. Surface patterns uncover two important aspects of the growth, i.e. carbon diffusion and stoichiometric requirement. Moreover, a new "stepdown" growth mode has been discovered. Via this mode, monolayer graphene domains can have an area of hundreds of square micrometers, while, most importantly, step bunching is avoided and the initial uniformly stepped SiC surf…
The growth of single layer graphene nanometer size domains by solid carbon source molecular beam epitaxy on hexagonal boron nitride (h-BN) flakes is demonstrated. Formation of single-layer graphene is clearly apparent in Raman spectra which display sharp optical phonon bands. Atomic-force microscope images and Raman maps reveal that the graphene grown depends on the surface morphology of the h-BN substrates. The growth is governed by the high mobility of the carbon atoms on the h-BN surface, in a manner that is consistent with van der Waals epitaxy. The successful growth of graphene layers dep…
We demonstrate molecular beam growth of graphene on biotite mica substrates at temperatures below 1000°C. As indicated by optical and atomic force microscopy, evaporation of carbon from a high purity solid-state source onto biotite surface results in the formation of single-, bi-, and multilayer graphene with size in the micrometer regime. Graphene grown directly on mica surface is of very high crystalline quality with the defect density below the threshold detectable by Raman spectroscopy. The interaction between graphene and the mica substrate is studied by comparison of the Raman spectrosco…
The effect of contact architecture, graphene defect density and metal-semiconductor work function difference on resistivity of metal-graphene contacts have been investigated. An architecture with metal on the bottom of graphene is found to yield resistivities that are lower, by a factor of 4, and most consistent as compared to metal on top of graphene. Growth defects in graphene film were found to further reduce resistivity by a factor of 2. Using a combination of method and metal used, the contact resistivity of graphene has been decreased by a factor of 10 to 1200 +- 250 Ohm-um using Palladi…
A foundation of the modern technology that uses single-crystal silicon has been the growth of high-quality single-crystal Si ingots with diameters up to 12 inches or larger. For many applications of graphene, large-area high-quality (ideally of single-crystal) material will be enabling. Since the first growth on copper foil a decade ago, inch-sized single-crystal graphene has been achieved. We present here the growth, in 20 minutes, of a graphene film of 5 x 50 cm2 dimension with > 99% ultra-highly oriented grains. This growth was achieved by: (i) synthesis of sub-metre-sized single-crystal Cu…
We studied the growth of an epitaxial graphene monolayer on Ru(0001). The graphene monolayer covers uniformly the Ru substrate over lateral distances larger than several microns reproducing the structural defects of the Ru substrate. The graphene is rippled with a periodicity dictated by the difference in lattice parameter between C and Ru. The theoretical model predict inhomogeneities in the electronic structure. This is confirmed by measurements in real space by means of scanning tunnelling spectroscopy. We observe electron pockets at the higher parts of the ripples.
A detailed review of the literature for the last 5-10 years on epitaxial growth of graphene is presented. Both experimental and theoretical aspects related to growth on transition metals and on silicon carbide are thoroughly reviewed. Thermodynamic and kinetic aspects of growth on all these materials, where possible, are discussed. To make this text useful for a wider audience, a range of important experimental techniques that have been used over the last decade to grow (e.g. CVD, TPG and segregation) and characterize (STM, LEEM, etc.) graphene are reviewed, and a critical survey of the most i…
A bottom-up chemical vapor deposition (CVD) process for the growth of graphene nanomesh films is demonstrated. The process relies on silicon nanospheres to block nucleation sites for graphene CVD on copper substrates. These spheres are formed in a self-organized way through silicon diffusion through a 5 $μ$m copper layer on a silicon wafer coated with 400 nm of silicon nitride. The temperature during the growth process disintegrates the $Si_3$$N_4$ layer and silicon atoms diffuse to the copper surface, where they form the nanospheres. After graphene nanomesh growth, the Si nanospheres can be r…
Inspired by recent studies of various two-dimensional (2D) metals such as Au, Fe and Ag, we study the growth of two-dimensional gold patches in graphene pores by density-functional theory. We find that at room temperature gold atoms diffuse readily on top of both graphene and two-dimensional gold with energy barriers less than $0.5$ eV. Furthermore, gold atoms move without barriers from the top of graphene to its edge and from the top of 2D gold to its edge. The energy barriers are absent even at the interface of 2D gold and graphene, so that the gold atoms move effortlessly across the interfa…
Highly dendritic graphene crystals up to 0.25 mm in diameter are synthesized by low pressure chemical vapor deposition inside a copper enclosure. With their sixfold symmetry and fractal-like shape, the crystals resemble snowflakes. The evolution of the dendritic growth features is investigated for different growth conditions and surface diffusion is found to be the growth-limiting step responsible for the formation of dendrites. The electronic properties of the dendritic crystals are examined down to sub-Kelvin temperatures, showing a mobility of up to 6300 cm$^2$V$^{-1}$s$^{-1}$ and quantum H…
We observe that gold atoms deposited by physical vapor deposition onto few layer graphenes condense upon annealing to form nanoparticles with an average diameter that is determined by the graphene film thickness. The data are well described by a theoretical model in which the electrostatic interactions arising from charge transfer between the graphene and the gold particle limit the size of the growing nanoparticles. The model predicts a nanoparticle size distribution characterized by a mean diameter D that follows a scaling law D proportional to m^(1/3), where m is the number of carbon layers…
Graphene, a hexagonal sheet of $sp^2$-bonded carbon atoms, has extraordinary properties which hold immense promise for future nanoelectronic applications. Unfortunately, the popular preparation methods of micromechanical cleavage and chemical exfoliation of graphite do not easily scale up for application purposes. Epitaxial graphene provides an attractive alternative, though there are many challenges, not least of which is the absence of an understanding of the complex atomistic assembly kinetics of graphene. Here, we present a simple rate theory of epitaxial graphene growth on close-packed me…
We report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by x-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Transport measurements of exfoliated graphene after SrO deposition show a strong dependence between the Dirac point and Sr oxidation. Subsequently, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (0…
As a viable candidate for an all-carbon post-CMOS electronics revolution, epitaxial graphene has attracted significant attention. To realize its application potential, reliable methods for fabricating large-area single-crystalline graphene domains are required. A new way to synthesize high quality epitaxial graphene, namely "face-to-face" method, has been reported in this paper. The structure and morphologies of the samples are characterized by low-energy electron diffraction, atomic force microscopy, angle-resolved photoemission spectroscopy and Raman spectroscopy. The grown samples show bett…
Using high temperature annealing conditions with a graphite cap covering the C-face of an 8deg off-axis 4H-SiC sample, large and homogeneous single epitaxial graphene layers have been grown. Raman spectroscopy shows evidence of the almost free-standing character of these monolayer graphene sheets, which was confirmed by magneto-transport measurements. We find a moderate p-type doping, high carrier mobility and half integer Quantum Hall effect typical of high quality graphene samples. This opens the way to a fully compatible integration of graphene with SiC devices on the wafers that constitute…
Atomically precise tailoring of graphene can enable unusual transport pathways and new nanometer-scale functional devices. Here we describe a recipe for the controlled production of highly regular "5-5-8" line defects in graphene by means of simultaneous electron irradiation and Joule heating by applied electric current. High-resolution transmission electron microscopy reveals individual steps of the growth process. Extending earlier theoretical work suggesting valley-discriminating capabilities of a graphene 5-5-8 line defect, we perform first-principles calculations of transport and find a s…
We report graphene films composed mostly of one or two layers of graphene grown by controlled carbon precipitation on the surface of polycrystalline Ni thin films during atmospheric chemical vapor deposition(CVD). Controlling both the methane concentration during CVD and the substrate cooling rate during graphene growth can significantly improve the thickness uniformity. As a result, one- or two- layer graphene regions occupy up to 87% of the film area. Single layer coverage accounts for 5-11% of the overall film. These regions expand across multiple grain boundaries of the underlying polycrys…
Ordered atomic-scale superlattices on surface hold great interest both for basic science and for potential applications in advanced technology. However, controlled fabrication of superlattices down to atomic scale has proven exceptionally challenging. Here we demonstrate the segregation-growth and self-organization of ordered S atomic superlattices confined at the interface between graphene and S-rich Cu substrates. Scanning tunneling microscope (STM) studies show that, by finely controlling the growth temperature, we obtain well-ordered S (sub)nanometer-cluster superlattice and monoatomic sup…
Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to term…
Realization of post-CMOS graphene electronics requires production of semiconducting graphene, which has been a labor-intensive process. We present tailoring of silicon carbide crystals via conventional photolithography and microelectronics processing to enable templated graphene growth on 4H-SiC{1-10n} (n = 8) crystal facets rather than the customary {0001} planes. This allows self-organized growth of graphene nanoribbons with dimensions defined by those of the facet. Preferential growth is confirmed by Raman spectroscopy and high-resolution transmission electron microscopy (HRTEM) measurement…
The development of wafer-scale continuous single-crystal graphene layers is key in view of its prospective applications. To this end, here we pave the way for a graphene growth model in the framework of the Langmuir adsorption theory and two dimensional crystallization. In specific, we model the nucleation and growth of graphene on copper using methane as carbon precursor. The model leads to identification of the range of growth parameters (temperature and gas pressures) that uniquely entails the final surface coverage of graphene. This becomes an invaluable tool to address the fundamental pro…
Large-area graphene is a new material with properties that make it desirable for advanced scaled electronic devices1. Recently, chemical vapor deposition (CVD) of graphene and few-layer graphene using hydrocarbons on metal substrates such as Ni and Cu has shown to be a promising technique2-5. It has been proposed in recent publications that graphene growth on Ni occurs by C segregation2 or precipitation3, while that on Cu is by surface adsorption5. In this letter, we used a carbon isotope labeling technique to elucidate the growth kinetics and unambiguously demonstrate that graphene growth on …
The growth process of single layer graphene with and without substrate is investigated using ab initio, finite temperature molecular dynamic calculations within density functional theory. An understanding of the epitaxial graphene growth mechanisms in the atomic level is provided by exploring the transient stages which occur at the growing edges of graphene. These stages are formation and collapse of large carbon rings together with the formation and healing of Stone-Wales like pentagon-heptagon defects. The activation barriers for the healing of these growth induced defects on various substra…
The growth of graphene by catalytic decomposition of ethylene on Cu(111) in an ultra-high vacuum system was investigated with low energy electron diffraction, low energy electron microscopy, and atomic force microscopy. Attempts to form a graphene overlayer using ethylene at pressures as high as 10 mTorr and substrate temperatures as high as 900 $^\circ$C resulted in almost no graphene growth. By using an argon overpressure, the growth of epitaxial graphene on Cu(111) was achieved. The suppression of graphene growth without the use of an argon overpressure is attributed to Cu sublimation at el…
In graphene growth, island symmetry can become lower than the intrinsic symmetries of both graphene and the substrate. First-principles calculations and Monte Carlo modeling explain the shapes observed in our experiments and earlier studies for various metal surface symmetries. For equilibrium shape, edge energy variations $δE$ manifest in distorted hexagons with different ground-state edge structures. In growth or nucleation, energy variation enters exponentially as $\sim e^{δE / k_{B} T}$, strongly amplifying the symmetry breaking, up to completely changing the shapes to triangular, ribbon-l…
Graphene has attracted a lot of research interests due to its exotic properties and a wide spectrum of potential applications. Chemical vapor deposition (CVD) from gaseous hydrocarbon sources has shown great promises for large-scale graphene growth. However, high growth temperature, typically 1000°C, is required for such growth. Here we demonstrate a revised CVD route to grow graphene on Cu foils at low temperature, adopting solid and liquid hydrocarbon feedstocks. For solid PMMA and polystyrene precursors, centimeter-scale monolayer graphene films are synthesized at a growth temperature down …
An in vacuo thermal desorption process has been accomplished to form epitaxial graphene (EG) on 4H- and 6H-SiC substrates using a commercial chemical vapor deposition reactor. Correlation of growth conditions and the morphology and electrical properties of EG are described. Raman spectra of EG on Si-face samples were dominated by monolayer thickness. This approach was used to grow EG on 50 mm SiC wafers that were subsequently fabricated into field effect transistors with fmax of 14 GHz.
The direct growth of graphene on semiconducting or insulating substrates might help to overcome main drawbacks of metal-based synthesis, like metal-atom contaminations of graphene, transfer issues, etc. Here we present the growth of graphene on n-doped semiconducting Ge(110) by using an atomic carbon source and the study of the structural and electronic properties of the obtained interface. We found that graphene interacts weakly with the underlying Ge(110) substrate that keeps graphene's electronic structure almost intact promoting this interface for future graphene-semiconductor applications…
We developed a method of precise isotope labeling to visualize the continuous growth of graphene by chemical vapor deposition (CVD). This method allows us to see in real time the growth of graphene monocrystals at a resolution of a few seconds. This technique is used to extract the anisotropic growth rates, the formation of dendrites, and the dependence on adsorption area of methane on copper. We obtain a physical picture of the growth dynamics of graphene and its dependence on various parameters. Finally, our method is relevant to other CVD grown materials.
In recent years, graphene growth optimization has been one of the key routes towards large-scale, high-quality graphene production. We have measured in-situ residual gas content during epitaxial graphene growth on silicon carbide (SiC) to find detrimental factors of epitaxial graphene growth. The growth conditions in high vacuum and purified argon are compared. The grown epitaxial graphene is studied by Raman scattering mapping and mechanical strain, charge density, number of graphene layers and graphene grain size are evaluated. Charge density and carrier mobility has been studied by Hall eff…
Fabrication of graphene devices is often hindered by incompatibility between the silicon technology and the methods of graphene growth. Exfoliation from graphite yields excellent films but is good mainly for research. Graphene grown on metal has a technological potential but requires mechanical transfer. Growth by SiC decomposition requires a temperature budget exceeding the technological limits. These issues could be circumvented by growing graphene directly on insulator, implying Van der Waals growth. During growth, the insulator acts as a support defining the growth plane. In the device, it…
Graphene forms from a relatively dense, tightly-bound C-adatom gas, when elemental C is deposited on or segregates to the Ru(0001) surface. Nonlinearity of the graphene growth rate with C adatom density suggests that growth proceeds by addition of C atom clusters to the graphene edge. The generality of this picture has now been studied by use of low-energy electron microscopy (LEEM) to observe graphene formation when Ru(0001) and Ir(111) surfaces are exposed to ethylene. The finding that graphene growth velocities and nucleation rates on Ru have precisely the same dependence on adatom concentr…
We have determined the growth mode of graphene on SiC(0001) and SiC(000-1) using ultra-thin, isotopically-labeled Si13C `marker layers' grown epitaxially on the Si12C surfaces. Few-layer graphene overlayers were formed via thermal decomposition at elevated temperature. For both surface terminations (Si-face and C-face), we find that the 13C is located mainly in the outermost graphene layers, indicating that, during decomposition, new graphene layers form underneath existing ones.
Although the corresponding carbon-metal interactions can be very different, a similar nonlinear growth behavior of graphene has been observed for different metal substrates. To understand this interesting experimental observation, a multiscale $\lq\lq$standing-on-the-front" kinetic Monte Carlo study is performed. An extraordinary robust geometry effect is identified, which solely determines the growth kinetics and makes the details of carbon-metal interaction not relevant at all. Based on such a geometry-determined mechanism, epitaxial growth behavior of graphene can be easily predicted in man…
We set up an evolutionary algorithm combined with density functional tight-binding (DFTB) calculations to investigate hydrogen adsorption on flat graphene and graphene monolayers curved over substrate steps. During the evolution, candidates for the new generations are created by adsorption of an additional hydrogen atom to the stable configurations of the previous generation, where a mutation mechanism is also incorporated. Afterwards a two-stage selection procedure is employed. Selected candidates act as the parents of the next generation. In curved graphene, the evolution follows a similar p…
Germanium is emerging as the substrate of choice for the growth of graphene in CMOS-compatible processes. For future application in next generation devices the accurate control over the properties of high-quality graphene synthesized on Ge surfaces, such as number of layers and domain size, is of paramount importance. Here we investigate the role of the process gas flows on the CVD growth of graphene on Ge(100). The quality and morphology of the deposited material is assessed by using microRaman spectroscopy, x-ray photoemission spectroscopy, scanning electron and atomic force microscopies. We…
Understanding the influence that copper substrate surface symmetry and oxygen impurities have on the growth of graphene by chemical vapor deposition is important for developing techniques for producing high quality graphene. Therefore, we have studied the growth of graphene by catalytic decomposition of ethylene in an ultra-high vacuum chamber on both a clean Cu(100) surface and a Cu(100) surface pre-dosed with a layer of chemisorbed oxygen. The crystal structure of the graphene films was characterized with \emph{in-situ} low energy electron diffraction. By heating the clean Cu(100) substrate …
Strain can be used as an alternate way to tune the electronic properties of graphene. Here we demonstrate that it is possible to tune the uniform strain of graphene simply by changing the chemical vapor deposition growth temperature of graphene on copper. Due to the cooling of the graphene on copper system, we can induce a uniform compressive strain on graphene. The strain is analyzed by Raman spectroscopy, where a shift in the 2D peak is observed and compared to our ab initio calculations of the graphene on copper system as a function of strain.
Using first-principles calculations within density functional theory, we study the energetics and kinetics of carbon nucleation in the early stages of epitaxial graphene growth on three representative stepped metal surfaces: Ir(111), Ru(0001), and Cu(111). We find that on the flat surfaces of Ir(111) and Ru(0001), two carbon atoms repel each other, while they prefer to form a dimer on Cu(111). Moreover, the step edges on Ir and Ru surfaces cannot serve as effective trapping centers for single carbon adatoms, but can readily facilitate the formation of carbon dimers. These contrasting behaviors…
Graphene was epitaxially grown on both the C- and Si-faces of 4H- and 6H-SiC(0001) under an argon atmosphere and under high vacuum conditions. Following growth, samples were imaged with Nomarski interference contrast and atomic force microscopies and it was found that growth under argon led to improved morphologies on the C-face films but the Si-face films were not significantly affected. Free carrier transport studies were conducted through Hall effect measurements, and carrier mobilities were found to increase and sheet carrier densities were found to decrease for those films grown under arg…
The growth of para-sexiphenyl (6P) thin films as a function of substrate temperature on Ir{111} supported graphene flakes has been studied in real-time with Low Energy Electron Microscopy (LEEM). Micro Low Energy Electron Diffraction (μLEED) has been used to determine the structure of the different 6P features formed on the surface. We observe the nucleation and growth of a wetting layer consisting of lying molecules in the initial stages of growth. Graphene defects -- wrinkles -- are found to be preferential sites for the nucleation of the wetting layer and of the 6P needles that grow on top …
A seed layer-free growth of HfO$_2$ on commercially available CVD graphene from various suppliers is investigated. It is revealed that the samples of monolayer graphene transferred from Cu to SiO$_2$/Si substrates have different coverage with bi- and multi-layer graphene islands. We find that the distribution and number of such islands impact the nucleation and growth of HfO$_2$ by CVD. In particular, we show that the edges and surface of densely distributed bi-layer graphene islands provide good nucleation sites for conformal CVD HfO$_2$ layers. Dielectric constant of 16 is extracted from mea…
We have used low-energy electron microscopy and diffraction to examine the significance of lattice orientation in graphene growth on Cu(001). Individual graphene domains undergo anisotropic growth on the Cu surface, and develop into lens shapes with their long axes roughly aligned with the Cu<100> in-plane directions. The long axis of a lens-shaped domain is only rarely oriented along a C<11> direction, suggesting that carbon attachment at "zigzag" graphene island edges is unfavorable. A kink-mediated adatom attachment process is consistent with the behavior observed here and reported in the l…
We demonstrate hydrogen assisted growth of high quality epitaxial graphene on the C-face of 4H-SiC. Compared with the conventional thermal decomposition technique, the size of the growth domain by this method is substantially increased and the thickness variation is reduced. Based on the morphology of epitaxial graphene, the role of hydrogen is revealed. It is found that hydrogen acts as a carbon etchant. It suppresses the defect formation and nucleation of graphene. It also improves the kinetics of carbon atoms via hydrocarbon species. These effects lead to increase of the domain size and the…
Graphene-metal interface as one of the interesting graphene-based objects attracts much attention from both application and fundamental science points of view. This paper gives a timely review of the recent experimental works on the growth and the electronic properties of the graphene-metal interfaces. This work makes a link between huge amount of experimental and theoretical data allowing one to understand the influence of the metallic substrate on the electronic properties of a graphene overlayer and how its properties can be modified in a controllable way. The further directions of studies …
We present a new fabrication method for epitaxial graphene on SiC which enables the growth of ultra-smooth defect- and bilayer-free graphene sheets with an unprecedented reproducibility, a necessary prerequisite for wafer-scale fabrication of high quality graphene-based electronic devices. The inherent but unfavorable formation of high SiC surface terrace steps during high temperature sublimation growth is suppressed by rapid formation of the graphene buffer layer which stabilizes the SiC surface. The enhanced nucleation is enforced by decomposition of polymer adsorbates which act as a carbon …
The growth of single and multilayer graphene nano-flakes on MgO and ZrO2 at low temperatures is shown through transmission electron microscopy. The graphene nano-flakes are ubiquitously anchored at step edges on MgO (100) surfaces. Density functional theory investigations on MgO (100) indicate C2H2 decomposition and carbon adsorption at step-edges. Hence, both the experimental and theoretical data highlight the importance of step sites for graphene growth on MgO.
Principal structural defects in graphene layers, synthesized on a carbon-terminated face, i.e. the SiC(000) face of a 4H-SiC substrate, are investigated using microscopic methods. Results of high-resolution transmission electron microscopy (HRTEM) reveal their atomic arrangement. Mechanism of such defects creation, directly related to the underlying crystallographic structure of the SiC substrate, is elucidated. The connection between the 4H-SiC(000) surface morphology, including the presence of the single atomic steps, the sequences of atomic steps, and also the macrosteps, and the correspond…
Plasma enhanced chemical vapor deposition (PECVD) techniques have been shown to be an efficient method to achieve single-step synthesis of high-quality monolayer graphene (MLG) without the need of active heating. Here we report PECVD-growth of single-crystalline hexagonal bilayer graphene (BLG) flakes and mm-size BLG films with the interlayer twist angle controlled by the growth parameters. The twist angle has been determined by three experimental approaches, including direct measurement of the relative orientation of crystalline edges between two stacked monolayers by scanning electron micros…
A basic kinetic model that incorporates a coupled dynamics of the carbon atoms and dimers on a copper surface is used to compute growth of a single-layer graphene island. The speed of the island's edge advancement on Cu[111] and Cu[100] surfaces is computed as a function of the growth temperature and pressure. Spatially resolved concentration profiles of the atoms and dimers are determined, and the contributions provided by these species to the growth speed are discussed. Island growth in the conditions of a thermal cycling is studied.
Using in situ low-energy electron microscopy and density functional theory, we studied the growth structure and work function of bilayer graphene on Pd(111). Low-energy electron diffraction analysis established that the two graphene layers have multiple rotational orientations relative to each other and the substrate plane. We observed heterogeneous nucleation and simultaneous growth of multiple, faceted layers prior to the completion of second layer. We propose that the facetted shapes are due to the zigzag-terminated edges bounding graphene layers growing under the larger overlying layers. W…
From both fundamental and technical points of view, a precise control of the layer number of graphene samples is very important. To reach this goal, atomic scale mechanisms of multilayer graphene growth on metal surfaces should be understood. Although it is a geometrically favorable pathway to transport carbon species to interface and then form a new graphene layer there, penetration of a graphene overlayer is not a chemically straightforward process. In this study, the possibility of different active species to penetrate a graphene overlayer on Cu(111) surface is investigated based on first p…
Direct growth of flat micrometer-sized bilayer graphene islands in between molybdenum disulfide sheets is achieved by chemical vapor deposition of ethylene at about 800 °C. The temperature assisted decomposition of ethylene takes place mainly at molybdenum disulfide step edges. The carbon atoms intercalate at this high temperature, and during the deposition process, through defects of the molybdenum disulfide surface such as steps and wrinkles. Post growth atomic force microscopy images reveal that circular flat graphene islands have grown at a high yield. They consist of two graphene layers s…
Graphene has recently been attracting considerable interest because of its exceptional conductivity, mechanical strength, thermal stability, etc. Graphene-based devices exhibit high potential for applications in flexible electronics, optoelectronics, and energy harvesting. In this paper, we review various growth strategies including metal-catalyzed transfer-free growth and direct-growth of graphene on flexible insulating substrates which are major issues for avoiding the complicated transfer process that cause graphene defects, residues, tears and performance degradation of its functional devi…
Applying time-dependent photoemission we unravel the graphene growth process on a metallic surface by chemical vapor deposition (CVD). Graphene CVD growth is in stark contrast to the standard growth process of two--dimensional films because it is self-limiting and stops as soon as a monolayer graphene has been synthesized. Most importantly, a novel phase of metastable graphene was discovered that is characterized by permanent and simultaneous construction and deconstruction. The high quality and large area graphene flakes are characterized by angle-resolved photoemission proofing that they are…
At a single atom thick, it is challenging to distinguish graphene from its substrate using conventional techniques. In this paper we show that friction force microscopy (FFM) is a simple and quick technique for identifying graphene on a range of samples, from growth substrates to rough insulators. We show that FFM is particularly effective for characterising graphene grown on copper where it can correlate the graphene growth to the three-dimensional surface topography and map the crystallographic orientation of the graphene nondestructively, reproducibly and at high resolution. We expect FFM t…
