Journal
CHEMISTRY OF MATERIALS
Volume 24, Issue 20, Pages 3906-3915Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm301993z
Keywords
graphene; growth; PAHs; coronene; pentacene; rubrene; first-principles
Funding
- Research Grants Council of Hong Kong [CUHK2/CRF/08, CUHK4179/10E]
- University Grants Committee of the Hong Kong Special Administrative Region, China [AoE/P-03/08]
- National Science Foundation of China [60990314, 60928009]
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Recent studies show that, at the initial stage of chemical vapor deposition (CVD) of graphene, the isolated carbon monomers will form defective carbon clusters with pentagons that degrade the quality of synthesized graphene. To circumvent this problem, we demonstrate that high-quality centimeter-sized graphene sheets can be synthesized on Cu foils by a self-assembled approach from defect-free polycyclic aromatic hydrocarbons (PAHs) in a high vacuum (HV) chamber without hydrogen. Different molecular motifs, namely coronene, pentacene, and rubrene, can lead to significant difference in the quality of resulting graphene. For coronene, monolayer graphene flakes with an adequate quality can be achieved at a growth temperature as low as 550 degrees C. For the graphene obtained at 1000 degrees C, transport measurements performed on back-gated field-effect transistors (FETs) with large channel lengths (similar to 30 mu m) exhibit a carrier mobility up to similar to 5300 cm(2) V-1 s(-1) sat room temperature. The underlying growth mechanism, which mainly involves surface-mediated nucleation process of dehydrogenated PAHs rather than segregation or precipitation process of small carbon species decomposed from the precursors, has been systematically investigated through the first-principles calculations. Our findings pave the way for optimizing selection of solid carbon precursors and open up a new route for graphene synthesis.
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