RESUMEN
Many scientific and engineering efforts have been made to realize graphene electronics by fully utilizing intrinsic properties of ideal graphene for last decades. The most technical huddles come from the absence of wafer-scale graphene with a single-crystallinity on dielectric substrates. Here, we report an epitaxial growth of single-crystalline monolayer graphene directly on a single-crystalline dielectric SiON-SiC(0001) with a full coverage via epitaxial chemical vapor deposition (CVD) without metal catalyst. The dielectric surface of SiON provides atomically flat and chemically inert interface by passivation of dangling bonds, which keeps intrinsic properties of graphene. Atomic structures with a clean interface, full coverage of single-crystalline monolayer, and the epitaxy of graphene on SiON were confirmed macroscopically by mapping low energy electron diffraction (LEED) and Raman spectroscopy, and atomically by scanning tunneling microscopy (STM). Both of measured and calculated local density of states (LDOS) exhibit a symmetric and sharp Dirac cone with a Dirac point located at a Fermi level. Our method provides a route to utilize a single-crystalline dielectric substrate for ideal graphene growth for future applications.
RESUMEN
Future applications of graphene rely highly on the production of large-area high-quality graphene, especially large single-crystalline graphene, due to the reduction of defects caused by grain boundaries. However, current large single-crystalline graphene growing methodologies are suffering from low growth rate and as a result, industrial graphene production is always confronted by high energy consumption, which is primarily caused by high growth temperature and long growth time. Herein, a new growth condition achieved via ethane being the carbon feedstock to achieve low-temperature yet rapid growth of large single-crystalline graphene is reported. Ethane condition gives a growth rate about four times faster than methane, achieving about 420 µm min-1 for the growth of sub-centimeter graphene single crystals at temperature about 1000 °C. In addition, the temperature threshold to obtain graphene using ethane can be reduced to 750 °C, lower than the general growth temperature threshold (about 1000 °C) with methane on copper foil. Meanwhile ethane always keeps higher graphene growth rate than methane under the same growth temperature. This study demonstrates that ethane is indeed a potential carbon source for efficient growth of large single-crystalline graphene, thus paves the way for graphene in high-end electronical and optoelectronical applications.
RESUMEN
The symmetry of graphene is usually determined by a low-energy electron diffraction (LEED) method when the graphene is on the conductive substrates, but LEED cannot handle graphene transferred to SiO2/Si substrates due to the charging effect. While transmission electron microscopy can generate electron diffraction on post-transferred graphene, this method is too localized. Herein, we employed an azimuthal reflection high-energy electron diffraction (RHEED) method to construct the reciprocal space mapping and determine the symmetry of wafer-size graphene both pre- and post-transfer. In this work, single-crystalline Cu(111) films were prepared on sapphire(0001) and spinel(111) substrates with sputtering. Then the graphene was epitaxially grown on single-crystalline Cu(111) films with a low pressure chemical vapor deposition. The reciprocal space mapping using azimuthal RHEED confirmed that the graphene grown on Cu(111) films was single-crystalline, no matter the form of the monolayer or multilayer structure. While the Cu(111) film grown on sapphire(0001) may occasionally consist of 60° in-plane rotational twinning, the reciprocal space mapping revealed that the in-plane orientation of graphene grown atop was not affected. The proposed method for checking the crystalline integrity of the post-transferred graphene sheets is an important step in the realization of the graphene as a platform to fabricate electronic and optoelectronic devices.
RESUMEN
Atomically thin single crystals, without grain boundaries and associated defect clusters, represent ideal systems to study and understand intrinsic defects in materials, but probing them collectively over large area remains nontrivial. In this study, the authors probe nanoscale mass transport across large-area (≈0.2 cm2 ) single-crystalline graphene membranes. A novel, polymer-free picture frame assisted technique, coupled with a stress-inducing nickel layer is used to transfer single crystalline graphene grown on silicon carbide substrates to flexible polycarbonate track etched supports with well-defined cylindrical ≈200 nm pores. Diffusion-driven flow shows selective transport of ≈0.66 nm hydrated K+ and Cl- ions over ≈1 nm sized small molecules, indicating the presence of selective sub-nanometer to nanometer sized defects. This work presents a framework to test the barrier properties and intrinsic quality of atomically thin materials at the sub-nanometer to nanometer scale over technologically relevant large areas, and suggests the potential use of intrinsic defects in atomically thin materials for molecular separations or desalting.
RESUMEN
Wafer-sized single-crystalline Cu (100) surface can be readily achieved on stacked polycrystalline Cu foils via simple oxygen chemisorption-induced reconstruction, enabling fast growth of large-scale millimeter-sized single-crystalline graphene arrays under molecular flow. The maximum growth rate can reach 300 µm min-1 , several orders of magnitude higher than previously reported values for millimeter-sized single-crystalline graphene growth on Cu foils.
RESUMEN
A second passivation and a multistage carbon-source supply (CSS) allow a 50-fold enhancement of the growth rate of large single-crystalline graphene with a record growth rate of 101 µm min(-1) , almost 10 times higher than for pure copper. To this end the CSS is tailored at separate stages of graphene growth on copper foil, combined with an effective suppression of new spontaneous nucleation via second passivation.