Residue-free suspended graphene transferred by perforated template.

A residue-free transfer method for graphene is proposed in this study, especially for the fabrication of suspended structures. Using perforated polymer templates, graphene can be precisely transferred onto the specific position in the perforated target SiO2/Si substrates without the need for polymer removal and the subsequent thermal annealing process. The surface of the transferred graphene by the proposed method was analyzed and corroborated via Raman spectroscopy, Fourier transform infrared spectroscopy, transmission electron microscopy. The results of these analyses suggest that the graphene surface has no polymeric residues resulting from the transfer process. The proposed method provides a powerful approach for the transfer of 2D materials and it enables the exploitation of their suspended structures for device applications as well as the physical characterizations without worry on the effect of contaminants.

Ultrasoft silicon nanomembranes: thickness-dependent effective elastic modulus.

For decades, silicon (Si) has been widely used for the mass production of microelectronic circuits. Recently, as the thickness has been reduced to the nanometer scale, its application has expanded to various fields, including flexible and transparent 2D semiconductors. For the reliable and reproducible operation of such large flexible and transparent devices, obtaining precise information about the mechanical properties of low dimensional Si is crucial. Here, we demonstrate that a 2 nm-thick Si nanomembrane (NM) exhibits an extremely low Young's modulus of 3.25 GPa, a two-order smaller value than that of the bulk counterpart. Our systematic measurement of thickness-controlled Si NMs reveals the existence of significant size effect: The effective modulus rapidly changes from 180 GPa to 3.25 GPa under 25 nm to 2 nm thickness reduction. Our theoretical modeling successfully provides physical insight into the unique stiff-to-soft transition and extremely low modulus. We further demonstrate that the modulus of Si NMs can be tailored precisely via the control of surface morphology of membrane. This work therefore provides a comprehensive picture of how and why originally hard & stiff Si deforms so softly in the ultrathin 2D geometry, and proposes a new strategy to design the mechanical properties at nanoscale dimensions.

A graphene meta-interface for enhancing the stretchability of brittle oxide layers.

Oxide materials have recently attracted much research attention for applications in flexible and stretchable electronics due to their excellent electrical properties and their compatibility with established silicon semiconductor processes. Their widespread uptake has been hindered, however, by the intrinsic brittleness and low stretchability. Here we investigate the use of a graphene meta-interface to enhance the electromechanical stretchability of fragile oxide layers. Electromechanical tensile tests of indium tin oxide (ITO) layers on polymer substrates were carried out with in situ observations using an optical microscope. It was found that the graphene meta-interface reduced the strain transfer between the ITO layer and the substrate, and this behavior was well described using a shear lag model. The graphene meta-interface provides a novel pathway for realizing flexible and stretchable electronic applications based on oxide layers.

Double-layer CVD graphene as stretchable transparent electrodes.

The stretchability of CVD graphene with a large area is much lower than that of mechanically exfoliated pristine graphene owing to the intrinsic and extrinsic defects induced during its synthesis, etch-out of the catalytic metal, and the transfer processes. This low stretchability is the main obstacle for commercial application of CVD graphene in the field of flexible and stretchable electronics. In this study, artificially layered CVD graphene is suggested as a promising candidate for a stretchable transparent electrode. In contrast to single-layer graphene (SLG), multi-layer graphene has excellent electromechanical stretchability owing to the strain relaxation facilitated by sliding among the graphene layers. Macroscopic and microscopic electromechanical tensile tests were performed to understand the key mechanism for the improved stretchability, and crack generation and evolution were systematically investigated for their dependence on the number of CVD graphene layers during tensile deformation using lateral force microscopy. The stretchability of double-layer graphene (DLG) is much larger than that of SLG and is similar to that of triple-layer graphene (TLG). Considering the transmittance and the cost of transfer, DLG can be regarded as a suitable candidate for stretchable transparent electrodes.

Fracture characteristics of monolayer CVD-graphene.

We have observed and analyzed the fracture characteristics of the monolayer CVD-graphene using pressure bulge testing setup. The monolayer CVD-graphene has appeared to undergo environmentally assisted subcritical crack growth in room condition, i.e. stress corrosion cracking arising from the adsorption of water vapor on the graphene and the subsequent chemical reactions. The crack propagation in graphene has appeared to be able to be reasonably tamed by adjusting applied humidity and stress. The fracture toughness, describing the ability of a material containing inherent flaws to resist catastrophic failure, of the CVD-graphene has turned out to be exceptionally high, as compared to other carbon based 3D materials. These results imply that the CVD-graphene could be an ideal candidate as a structural material notwithstanding environmental susceptibility. In addition, the measurements reported here suggest that specific non-continuum fracture behaviors occurring in 2D monoatomic structures can be macroscopically well visualized and characterized.

Synthesis of CVD-graphene on rapidly heated copper foils.

Most chemical vapor deposition (CVD) systems used for graphene growth mainly employ convection and radiation heat transfer between the heating source and the metal catalyst in order to reach the activation temperature of the reaction, which in general leads to a long synthesis time and poor energy efficiency. Here, we report a highly time- and energy-efficient CVD setup, in which the metal catalyst (Cu) is designed to be physically contacted with a heating source to give quick heat transfer by conduction. The induced conduction heating enabled the usual effects of the pretreatment and annealing of Cu (i.e., annihilation of surface defects, impurities and contaminants) to be achieved in a significantly shorter time compared to conventional CVD. Notably, the rapid heating was observed to lead to larger grains of Cu with high uniformity as compared to the Cu annealed by conventional CVD, which are believed to be beneficial for the growth of high quality graphene. Through this CVD setup, bundles of high quality (∼252 Ω per square) and large area (over 16 inch) graphenes were able to be readily synthesized in 40 min in a significantly efficient way. When considering ease of scalability, high energy effectiveness and considerable productivity, our method is expected to be welcomed by industrialists.

Monatomic chemical-vapor-deposited graphene membranes bridge a half-millimeter-scale gap.

One of the main concerns in nanotechnology is the utilization of nanomaterials in macroscopic applications without losing their extreme properties. In an effort to bridge the gap between the nano- and macroscales, we propose a clever fabrication method, the inverted floating method (IFM), for preparing freestanding chemical-vapor-deposited (CVD) graphene membranes. These freestanding membranes were then successfully suspended over a gap a half-millimeter in diameter. To understand the working principle of IFM, high-speed photography and white light interferometry were used to characterize and analyze the deformation behaviors of the freestanding graphene membranes in contact with a liquid during fabrication. Some nanoscale configurations in the macroscopic graphene membranes were able to be characterized by simple optical microscopy. The proposed IFM is a powerful approach to investigating the macroscopic structures of CVD graphene and enables the exploitation of freestanding CVD graphene for device applications.

Dimensional dependence of phonon transport in freestanding atomic layer systems.

Due to the fast development of nanotechnology, we have the capability of manipulating atomic layer systems such as graphene, hexagonal boron nitride and dichalcogenides. The major concern in the 2-dimensional nanostructures is how to preserve their exceptional single-layer properties in 3-dimensional bulk structures. In this study, we report that the extreme phonon transport in graphene is highly affected by the graphitic layer stacking based on experimental investigation of the thermal conduction in few-layer graphene, 1-7 layers thick, suspended over holes of various diameters. We fabricate freestanding axisymmetric graphene structures without any perturbing substrate, and measure the in-plane transport property in terms of thermal conduction by using Raman spectroscopy. From the difference in susceptibility to substrate effect, size effect on hot-spot temperature variation and layer number dependence of thermal conductivity, we show that the graphitic membranes with 2 or more layers have characteristics similar to 3-dimensional graphite, which are very different from those of 2-dimensional graphene membranes. This implies that the scattering of out-of-plane phonons by interlayer atomic coupling could be a key mechanism governing the intrinsic thermal property.

Tensile testing of ultra-thin films on water surface.

The surface of water provides an excellent environment for gliding movement, in both nature and modern technology, from surface living animals such as the water strider, to Langmuir-Blodgett films. The high surface tension of water keeps the contacting objects afloat, and its low viscosity enables almost frictionless sliding on the surface. Here we utilize the water surface as a nearly ideal underlying support for free-standing ultra-thin films and develop a novel tensile testing method for the precise measurement of mechanical properties of the films. In this method, namely, the pseudo free-standing tensile test, all specimen preparation and testing procedures are performed on the water surface, resulting in easy handling and almost frictionless sliding without specimen damage or substrate effects. We further utilize van der Waals adhesion for the damage-free gripping of an ultra-thin film specimen. Our approach can potentially be used to explore the mechanical properties of emerging two-dimensional materials.