Low partial pressure chemical vapor deposition of graphene on copper

A systematic study of the Cu-catalyzed chemical vapor deposition of graphene under extremely low partial pressure is carried out. A carbon precursor supply of just P CH4∼ 0.009 mbar during the deposition favors the formation of large-area uniform monolayer graphene verified by Raman spectra. A diluted HNO 3 solution is used to remove Cu before transferring graphene onto SiO 2/Si substrates or carbon grids. The graphene can be made suspended over a ∼12 μm distance, indicating its good mechanical properties. Electron transport measurements show the graphene sheet resistance of ∼0.6 kΩ/□ at zero gate voltage. The mobilities of electrons and holes are ∼1800 cm 2/Vs at 4.2 K and ∼1200 cm 2/Vs at room temperature. © 2011 IEEE.

Controllable chemical vapor deposition of large area uniform nanocrystalline graphene directly on silicon dioxide

Metal-catalyst-free chemical vapor deposition (CVD) of large area uniform nanocrystalline graphene on oxidized silicon substrates is demonstrated. The material grows slowly, allowing for thickness control down to monolayer graphene. The as-grown thin films are continuous with no observable pinholes, and are smooth and uniform across whole wafers, as inspected by optical-, scanning electron-, and atomic force microscopy. The sp 2 hybridized carbon structure is confirmed by Raman spectroscopy. Room temperature electrical measurements show ohmic behavior (sheet resistance similar to exfoliated graphene) and up to 13 of electric-field effect. The Hall mobility is ∼40 cm 2/Vs, which is an order of magnitude higher than previously reported values for nanocrystalline graphene. Transmission electron microscopy, Raman spectroscopy, and transport measurements indicate a graphene crystalline domain size ∼10 nm. The absence of transfer to another substrate allows avoidance of wrinkles, holes, and etching residues which are usually detrimental to device performance. This work provides a broader perspective of graphene CVD and shows a viable route toward applications involving transparent electrodes. © 2012 American Institute of Physics.

Direct chemical vapor deposition of large-area carbon thin films on gallium nitride for transparent electrodes: A first attempt

Direct formation of large-area carbon thin films on gallium nitride by chemical vapor deposition without metallic catalysts is demonstrated. A high flow of ammonia is used to stabilize the surface of the GaN (0001)/sapphire substrate during the deposition at 950°C. Various characterization methods verify that the synthesized thin films are largely sp 2 bonded, macroscopically uniform, and electrically conducting. The carbon thin films possess optical transparencies comparable to that of exfoliated graphene. This paper offers a viable route toward the use of carbon-based materials for future transparent electrodes in III-nitride optoelectronics, such as GaN-based light emitting diodes and laser diodes. © 1988-2012 IEEE.

The parameter space of graphene chemical vapor deposition on polycrystalline Cu

A systematic study of the parameter space of graphene chemical vapor deposition (CVD) on polycrystalline Cu foils is presented, aiming at a more fundamental process rationale in particular regarding the choice of carbon precursor and mitigation of Cu sublimation. CH 4 as precursor requires H 2 dilution and temperatures ≥1000 °C to keep the Cu surface reduced and yield a high-quality, complete monolayer graphene coverage. The H 2 atmosphere etches as-grown graphene; hence, maintaining a balanced CH 4/H 2 ratio is critical. Such balance is more easily achieved at low-pressure conditions, at which however Cu sublimation reaches deleterious levels. In contrast, C 6H 6 as precursor requires no reactive diluent and consistently gives similar graphene quality at 100-150 °C lower temperatures. The lower process temperature and more robust processing conditions allow the problem of Cu sublimation to be effectively addressed. Graphene formation is not inherently self-limited to a monolayer for any of the precursors. Rather, the higher the supplied carbon chemical potential, the higher the likelihood of film inhomogeneity and primary and secondary multilayer graphene nucleation. For the latter, domain boundaries of the inherently polycrystalline CVD graphene offer pathways for a continued carbon supply to the catalyst. Graphene formation is significantly affected by the Cu crystallography; i.e., the evolution of microstructure and texture of the catalyst template form an integral part of the CVD process. © 2012 American Chemical Society.

Frame assisted H2O electrolysis induced H2 bubbling transfer of large area graphene grown by chemical vapor deposition on Cu

An improved technique for transferring large area graphene grown by chemical vapor deposition on copper is presented. It is based on mechanical separation of the graphene/copper by H2 bubbles during H2O electrolysis, which only takes a few tens of seconds while leaving the copper cathode intact. A semi-rigid plastic frame in combination with thin polymer layer span on graphene gives a convenient way of handling- and avoiding wrinkles and holes in graphene. Optical and electrical characterizations prove the graphene quality is better than that obtained by traditional wet etching transfer. This technique appears to be highly reproducible and cost efficient. © 2013 American Institute of Physics.

Tantalum-oxide catalysed chemical vapour deposition of single- and multi-walled carbon nanotubes

Tantalum-oxide thin films are shown to catalyse single- and multi-walled carbon nanotube growth by chemical vapour deposition. A low film thickness, the nature of the support material (best results with SiO2) and an atmospheric process gas pressure are of key importance for successful nanotube nucleation. Strong material interactions, such as silicide formation, inhibit nanotube growth. In situ X-ray photoelectron spectroscopy indicates that no catalyst reduction to Ta-metal or Ta-carbide occurs during our nanotube growth conditions and that the catalytically active phase is the Ta-oxide phase. Such a reduction-free oxide catalyst can be technologically advantageous. © 2013 The Royal Society of Chemistry.

Novel ZnO nanorod films by chemical solution deposition for planar device applications.

Smooth and continuous ZnO films consisting of densely packed ZnO nanorods (NRs), which can be used for electronic device fabrication, were synthesized using a hydro-thermo-chemical solution deposition method. Such devices would have the novelty of high performance, benefiting from the inherited unique properties of the nanomaterials, and can be fabricated on these smooth films using a conventional, low cost planar process. Photoluminescence measurements showed that the NR films have much stronger shallow donor to valence band emissions than those from discrete ZnO NRs, and hence have the potential for the development of ZnO light emission diodes and lasers, etc. The NR films have been used to fabricate large area surface acoustic wave devices by conventional photolithography. These demonstrated two well-defined resonant peaks and their potential for large area device applications. The chemical solution deposition method is simple, reproducible, scalable and economic. These NR films are suitable for large scale production on cost-effective substrates and are promising for various fields such as sensing systems, renewable energy and optoelectronic applications.

Near-field characterization of chemical vapor deposition graphene in the microwave regime

Near-field measurements were performed at X-band frequencies for graphene on copper microstrip transmission lines. An improvement in radiation of 0.88 dB at 10.2 GHz is exhibited from the monolayer graphene antenna which has dc sheet resistivity of 985 Ω/sq. Emission characteristics were validated via ab initio simulations and compared to empirical findings of geometrically comparable copper patches. This study contributes to the current knowledge of the electronic properties of graphene. © 2013 AIP Publishing LLC.

Diameter and wall number control of carbon nanotubes by chemical vapor deposition

We analyze the relationship between the average wall number (N) and the diameter (d) for carbon nanotubes (CNTs) grown by chemical vapour deposition. It is found that N depends linearly on d for diameters in the range of 2.5-10 nm, while single wall nanotubes predominate for diameters under about 2.1 nm. The linear relationship is found to depend somewhat on the growth conditions. It is also verified that the mean diameter depends on the diameter of the originating catalyst nanoparticle, and thus on the initial catalyst thickness where a thin film catalyst is used. This simplifies the characterisation of CNTs by electron microscopy. We also find a linear relationship between nanotube diameter and initial catalyst film thickness. © 2013 AIP Publishing LLC.

Co-catalytic absorption layers for controlled laser-induced chemical vapor deposition of carbon nanotubes.

The concept of co-catalytic layer structures for controlled laser-induced chemical vapor deposition of carbon nanotubes is established, in which a thin Ta support layer chemically aids the initial Fe catalyst reduction. This enables a significant reduction in laser power, preventing detrimental positive optical feedback and allowing improved growth control. Systematic study of experimental parameters combined with simple thermostatic modeling establishes general guidelines for the effective design of such catalyst/absorption layer combinations. Local growth of vertically aligned carbon nanotube forests directly on flexible polyimide substrates is demonstrated, opening up new routes for nanodevice design and fabrication.

A comparative study of plasma-enhanced chemical vapor gate dielectrics for solution-processed polymer thin-film transistor circuit integration

This paper considers plasma-enhanced chemical vapor deposited (PECVD) silicon nitride (SiNx) and silicon oxide (SiOx) as gate dielectrics for organic thin-film transistors (OTFTs), with solution-processed poly[5, 5′ -bis(3-dodecyl-2-thienyl)-2, 2′ -bithiophene] (PQT-12) as the active semiconductor layer. We examine transistors with SiNx films of varying composition deposited at 300 °C as well as 150 °C for plastic compatibility. The transistors show over 100% (two times) improvement in field-effect mobility as the silicon content in SiNx increases, with mobility (μFE) up to 0.14 cm2 /V s and on/off current ratio (ION / IOFF) of 108. With PECVD SiOx gate dielectric, preliminary devices exhibit a μFE of 0.4 cm2 /V s and ION / IOFF of 108. PQT-12 OTFTs with PECVD SiNx and SiOx gate dielectrics on flexible plastic substrates are also presented. These results demonstrate the viability of using PECVD SiN x and SiOx as gate dielectrics for OTFT circuit integration, where the low temperature and large area deposition capabilities of PECVD films are highly amenable to integration of OTFT circuits targeted for flexible and lightweight applications. © 2008 American Institute of Physics.

Effect of hydrogen dilution on the deposition of carbon-rich a-SiC:H films by the electron cyclotron resonance method

The deposition of hydrogenated amorphous silicon carbide (a-SiC:H) films from a mixture of silane, acetylene and hydrogen gas using the electron cyclotron resonance chemical vapour deposition (ECR-CVD) process is reported. The variation in the deposition and film characteristics such as the deposition rate, optical band gap and IR absorption as a function of the hydrogen dilution is investigated. The deposition rate increases to a maximum value of about 250 Å min-1 at a hydrogen dilution ratio of about 20 (hydrogen flow (sccm)/acetylene + silane flow (sccm)) and decreases in response to a further increase in the hydrogen dilution. There is no strong dependence of the optical band gap on the hydrogen dilution within the dilution range investigated (10-60) and the optical band gap calculated from the E04 method varied marginally from about 2.85 to 3.17 eV. The room temperature photoluminescence (PL) peak energy and intensity showed a prominent shift to a maximum value of about 2.17 eV corresponding to maximum PL intensity at a moderate hydrogen dilution of about 30. The PL intensity showed a strong dependence on the hydrogen dilution variation.