• Carbon letters
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• v.13 no.4
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• pp.205-211
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• 2012

Methanol as a carbon source in chemical vapor deposition (CVD) graphene has an advantage over methane and hydrogen in that we can avoid optimizing an etching reagent condition. Since methanol itself can easily decompose into hydrocarbon and water (an etching reagent) at high temperatures [1], the pressure and the temperature of methanol are the only parameters we have to handle. In this study, synthetic conditions for highly crystalline and large area graphene have been optimized by adjusting pressure and temperature; the effect of each parameter was analyzed systematically by Raman, scanning electron microscope, transmission electron microscope, atomic force microscope, four-point-probe measurement, and UV-Vis. Defect density of graphene, represented by D/G ratio in Raman, decreased with increasing temperature and decreasing pressure; it negatively affected electrical conductivity. From our process and various analyses, methanol CVD growth for graphene has been found to be a safe, cheap, easy, and simple method to produce high quality, large area, and continuous graphene films.

• Proceedings of the Korean Vacuum Society Conference
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• 2014.02a
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• pp.114.1-114.1
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• 2014

Copper is considered to be the most promising substrate for the growth of high-quality and large area graphene by chemical vapor deposition (CVD), in particular, on the (111) facet. Because the interactions between graphene and Cu substrates influence the orientation, quality, and properties of the synthesized graphene, we studied the interactions using angle-resolved photoemission spectroscopy. The evolution of both the Shockley surface state of the Cu(111) and the p band of the graphene was measured from the initial stage of CVD growth to the formation of a monolayer. Graphene growth was initiated along the Cu(111) lattice, where the Dirac band crossed the Fermi energy ($E_F$) at the K point without hybridization with the d-band of Cu. Then two rotated domains were additionally grown as the area covered with graphene became wider. The Dirac energy was about 0.4 eV and the energy of the Shockley surface state of Cu(111) shifted toward the $E_F$) by 0.15 eV upon graphene formation. These results indicate weak interactions between graphene and Cu, and that the electron transfer is limited to that between the Shockley surface state of Cu(111) and the p band of graphene. This weak interaction and slight lattice mismatch between graphene and Cu resulted in the growth of rotated graphene domains ($9.6^{\circ}$ and $8.4^{\circ}$), which showed no significant differences in the Dirac band with respect to different orientations. These rotated graphene domains resulted in grain boundaries which would hinder a large-sized single monolayer growth on Cu substrates.

• Proceedings of the Korean Vacuum Society Conference
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• 2013.08a
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• pp.130.2-130.2
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• 2013

Today, chemical vapor deposition (CVD) of hydrocarbon gases has been demonstrated as an attractive method to synthesize large-area graphene layers. However, special care should be taken to precisely control the resulting graphene layers in CVD due to its sensitivity to various process parameters. Therefore, a facile synthesis to grow graphene layers with high controllability will have great advantages for scalable practical applications. In order to simplify and create efficiency in graphene synthesis, the graphene growth by thermal annealing process has been discussed by several groups. However, the study on growth mechanism and the detailed structural and optoelectronic properties in the resulting graphene films have not been reported yet, which will be of particular interest to explore for the practical application of graphene. In this study, we report the growth of few-layer, large-area graphene films using rapid thermal annealing (RTA) without the use of intentional carbon-containing precursor. The instability of nickel films in air facilitates the spontaneous formation of ultrathin (<2~3 nm) carbon- and oxygen-containing compounds on a nickel surface and high-temperature annealing of the nickel samples results in the formation of few-layer graphene films with high crystallinity. From annealing temperature and ambient studies during RTA, it was found that the evaporation of oxygen atoms from the surface is the dominant factor affecting the formation of graphene films. The thickness of the graphene layers is strongly dependent on the RTA temperature and time and the resulting films have a limited thickness less than 2 nm even for an extended RTA time. The transferred films have a low sheet resistance of ~380 ${\Omega}/sq$, with ~93% optical transparency. This simple and potentially inexpensive method of synthesizing novel 2-dimensional carbon films offers a wide choice of graphene films for various potential applications.

• Journal of the Korean Vacuum Society
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• v.21 no.5
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• pp.279-285
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• 2012

We report on the measurements of electronic transport properties of CVD graphene placed on a pre-patterned substrate with periodic nano trenches. A strong anisotropy has been observed between the transport parallel and perpendicular to the trenches. Characteristically different weak localization corrections have been also observed when the transport was perpendicular to the trench, which is interpreted as due to a density inhomogeneity generated by the potential modulations.

• Proceedings of the Korean Vacuum Society Conference
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• 2012.08a
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• pp.181-181
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• 2012

Direct synthesis of graphene using a chemical vapor deposition (CVD) has been considered a facile way to produce large-area and uniform graphene film, which is an accessible method from an application standpoint. Hence, their fundamental understanding is highly required. Unfortunately, the CVD growth mechanism of graphene on Cu remains elusive and controversial. Here, we present the evidences for two different growth modes of graphene on Cu investigated by varying carbon feedstock (C2H2 and CH4) and working pressure. The number of uniform graphene layer grown by C2H2 increased with increasing its injection time. A combined secondary ion mass spectrometry (SIMS) and X-ray diffraction (XRD) study revealed a carbon-diffused Cu layer created below surface region of Cu substrate with the expansion of Cu lattice. The graphene on Cu was grown by the diffusion and precipitation mode not by the surface adsorption mode, because similar results were observed in graphene/Ni system. The carbon-diffused Cu layer was also observed after graphene growth under high CH4 pressure. Based on various previous results and ours, we have successfully found that there are two selective growth modes for graphene on Cu substrate, and a desired mode can be chosen by tuning working pressure corresponding to the kind of carbon feedstock. We believe that this finding will shed light on high quality graphene growth and its multifaceted applications.

• Proceedings of the Korean Vacuum Society Conference
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• 2010.02a
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• pp.39-39
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• 2010

There have been many efforts to utilize the outstanding properties of graphene for macroscopic applications such as transparent conducting films useful for flexible/stretchable electronics. However, the lack of efficient synthesis, transfer, and doping methods limited the scale and the quality needed for the practical production of graphene films. In this presentation, we introduce ultra-large scale (~30 inch) synthesis and roll-to-roll transfer of graphene films showing excellent electrical and physical properties suitable for practical applications. Considering the outstanding scalability/processibility of roll-to-roll and CVD methods and the extraordinary flexibility/conductivity of graphene films, we expect the commercial production and application electrodes replacing the use of ITO can be realized in near future.

• Proceedings of the Korean Vacuum Society Conference
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• 2013.02a
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• pp.207-207
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• 2013

기존의 그래핀 성장에 관한 연구는 열화학기상증착법(Chemical vapor deposition; CVD)을 이용한다. 그래핀 성장 제어 요소로는 촉매 기판인 전이 금속[Ru, Ir, Co, Re, Pt, Pd, Ni, Cu], 기판 전처리 과정, 수소/메탄 가스 혼합비, 작업 진공 상태, 기판온도[$800{\sim}1,000^{\circ}C$, 냉각 속도 등으로 보고 되고 있다. 그래핀 성장 원리는 Cu 촉매 기판에 메탄 가스를 $1,000^{\circ}C$ 온도에서 분해해서 탄소를 고용 시킨 후 급랭하는 도중에 석출되는 탄소에 의해 그래핀 시트가 형성되는 것으로 알려져 있다. 기존의 CVD를 열원을 이용할 경우 내부 챔버에 생기는 잠열에 의해 cooling profile의 제어가 용이하지 않다. 본 연구에서는 근적외선(Near Infrared; NIR) 열원을 이용한 CVD로 챔버 내부 잠열을 최소화하고, 냉각 공정을 Natural, Linear, Convex cooling type으로 디자인해서 cooling profile 제어가 그래핀 성장에 미치는 영향을 연구 하였다. 이렇게 성장된 그래핀을 임의의 기판(SiO2, Glass, PET film) 위에 습식방법으로 전이 시킨 후, 전기적 구조적 및 광학적 특성을 면저항(four-point probe), 전계방사 주사전자현미경(Field Emission Scanning Electron Microscope; FE-SEM), 마이크로 라만 분광법(Micro Raman spectroscopy) 및 광학현미경(optical microscope), 투과도(UV/Vis spectrometer)의 측정으로 잠열이 최소화된 NIR-CVD에서 cooling profile에 따른 그래핀 성장을 평가하였다.

• Proceedings of the Korean Vacuum Society Conference
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• 2016.02a
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• pp.280.2-280.2
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• 2016

The graphene, a single atomic sheet of graphite, has attracted tremendous interest owing to its novel properties including high intrinsic mobility, optical transparency and flexibility. However, for more diverse application of graphene devices, it is essential to tune its transport behavior by shifting Dirac Point (DP) of graphene. So, in the following context, we suggest a method to tune structural and electronic properties of graphene using atomic layer deposition. By atomic layer deposition of zinc oxide (ZnO) on graphene using 4-mercaptophenol as linker, we can fabricate n-doped graphene. Through ${\pi}-{\pi}$ stacking between chemically inert graphene and 4-mercaptophenol, conformal deposition of ZnO on graphene was enabled. The electron mobility of graphene TFT increased more than 3 times without considerably decreasing the hole mobility, compared to the pristine graphene. Also, it has high air stability. This ZnO doping method by atomic layer deposition can be applicable to large scale array of CVD graphene TFT.

• Proceedings of the Korean Vacuum Society Conference
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• 2012.08a
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• pp.105-105
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• 2012

We have developed a photoemission-assisted plasma-enhanced chemical vapor deposition (PAPE-CVD) [1,2], in which photoelectrons emitting from the substrate surface irradiated with UV light ($h{\nu}$=7.2 eV) from a Xe excimer lamp are utilized as a trigger for generating DC discharge plasma as depicted in Fig. 1. As a result, photoemission-assisted plasma can appear just above the substrate surface with a limited interval between the substrate and the electrode (~10 mm), enabling us to suppress effectively the unintended deposition of soot on the chamber walls, to increase the deposition rate, and to decrease drastically the electric power consumption. In case of the deposition of DLC gate insulator films for the top-gate graphene channel FET, plasma discharge power is reduced down to as low as 0.01W, giving rise to decrease significantly the plasma-induced damage on the graphene channel [3]. In addition, DLC thickness can be precisely controlled in an atomic scale and dielectric constant is also changed from low ${\kappa}$ for the passivation layer to high ${\kappa}$ for the gate insulator. On the other hand, negative electron affinity (NEA) of a hydrogen-terminated diamond surface is attractive and of practical importance for PAPECVD, because the diamond surface under PAPE-CVD with H2-diluted (about 1%) CH4 gas is exposed to a lot of hydrogen radicals and therefore can perform as a high-efficiency electron emitter due to NEA. In fact, we observed a large change of discharge current between with and without hydrogen termination. It is noted that photoelectrons are emitted from the SiO2 (350 nm)/Si interface with 7.2-eV UV light, making it possible to grow few-layer graphene on the thick SiO2 surface with no transition layer of amorphous carbon by means of PAPE-CVD without any metal catalyst.

• Korean Journal of Materials Research
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• v.24 no.12
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• pp.694-699
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• 2014

We report the chemical vapor deposition growth characteristics of graphene on various catalytic metal substrates such as Ni, Fe, Ag, Au, and Pt. 50-nm-thick metal films were deposited on $SiO_2/Si$ substrates using dc magnetron sputtering. Graphene was synthesized on the metal/$SiO_2$/Si substrates with $CH_4$ gas (1 SCCM) diluted in mixed gases of 10% $H_2$ and 90 % Ar (99 SCCM) using inductively-coupled plasma chemical vapor deposition (ICP-CVD). The highest quality of graphene film was achieved on Ni and Fe substrates at $900^{\circ}C$ and 500 W of ICP power. Ni substrate seemed to be the best catalytic material among the tested materials for graphene growth because it required the lowest growth temperature ($600^{\circ}C$) as well as showing a low ICP power of 200W. Graphene films were successfully grown on Ag, Au, and Pt substrates as well. Graphene was formed on Pt substrate within 2 sec, while graphene film was achieved on Ni substrate over a period of 5 min of growth. These results can be understood as showing the direct CVD growth of graphene with a highly efficient catalytic reaction on the Pt surface.