Recent advances in chemical vapour deposition have led to the fabrication of large graphene sheets on metal foils for use in research and development. However, further breakthroughs are required in the way these graphenes are transferred from their growth substrates onto the final substrate. Although various methods have been developed, as yet there is no general way to reliably transfer graphene onto arbitrary surfaces, such as 'soft' ones. Here, we report a method that allows the graphene to be transferred with high fidelity at the desired location on almost all surfaces, including fragile polymer thin films and hydrophobic surfaces. The method relies on a sacrificial 'self-releasing' polymer layer placed between a conventional polydimethylsiloxane elastomer stamp and the graphene that is to be transferred. This self-releasing layer provides a low work of adhesion on the stamp, which facilitates delamination of the graphene and its placement on the new substrate. To demonstrate the generality and reliability of our method, we fabricate high field-strength polymer capacitors using graphene as the top contact over a polymer dielectric thin film. These capacitors show superior dielectric breakdown characteristics compared with those made with evaporated metal top contacts. Furthermore, we fabricate low-operation-voltage organic field-effect transistors using graphene as the gate electrode placed over a thin polymer gate dielectric layer. We finally demonstrate an artificial graphite intercalation compound by stacking alternate monolayers of graphene and 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ). This compound, which comprises graphene sheets p-doped by partial hole transfer from the F4TCNQ, shows a high and remarkably stable hole conductivity, even when heated in the presence of moisture.
Although all graphites share the same idealized chemical structure, marked differences in fact exist between their reactivities, such as the propensity for oxidation, that need to be taken into consideration for the development of applications. Here we show that five different commercially sourced natural and synthetic graphites differ significantly in their response to a modified Staudenmaier oxidation that produces substoichiometric graphene oxides (sub-GOx). The dominant oxidation product is hydroxyl groups, which can be dehydrate to epoxy groups under mild heating even below 120 °C. The extent of oxidation correlates broadly with the defect band intensity in the starting graphites as measured by Raman spectroscopy. FTIR shows there is a significant concentration of H defects at the % atom level. The results suggest that defects in the graphite plane are more prevalent than previously thought. Finally, the properties of the thermally reduced sub-GOx are also different. The product from the least defective starting graphite ultimately exhibits the lowest activation energies for both electron and hole transport, of the order of 10 μeV below 25 K, that is characteristic of band-like transport. These results are important because they show that the quality of the starting graphite significantly affects the properties of the derived products.
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