We report catalyst-free direct synthesis of vertical graphene nanosheets (VGNs) on SiO2/Si and quartz substrates using microwave electron cyclotron resonance - plasma enhanced chemical vapor deposition. The evolution of VGNs is studied systematically at different growth stages. Raman analysis as a function of growth time reveals that two different disorder-induced competing mechanisms contributing to the defect band intensity. The VGNs grown on SiO2/Si substrates predominantly consists of both vacancy-like and hopping defects. On the other hand, the VGNs grown on quartz substrates contain mainly boundary-like defects. XPS studies also corroborate Raman analysis in terms of defect density and vacancy-like defects for the VGNs grown on SiO2/Si substrates. Moreover, the grown VGNs exhibit a high optical transmittance from 95 to 78 % at 550 nm and the sheet resistance varies from 30 to 2.17 kohms/square depending on growth time.Comment: 19 pages, 8 figures, 1 table; Accepted in Journal of Raman Spectroscopy (2014

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Applications of plasma-produced vertically oriented graphene nanosheets (VGNs) rely on their unique structure and morphology, which can be tuned by the process parameters to understand the growth mechanism. Here, we report on the effect of the key process parameters such as deposition temperature, discharge power and distance from plasma source to substrate on the catalyst-free growth of VGNs in microwave plasmas. A direct evidence for the initiation of vertical growth through nanoscale graphitic islands is obtained from the temperature-dependent growth rates where the activation energy is found to be as low as 0.57 eV. It is shown that the growth rate and the structural quality of the films could be enhanced by (a) increasing the substrate temperature, (b) decreasing the distance between the microwave plasma source and the substrate, and (c) increasing the discharge power. The correlation between the wetting characteristics, morphology and structural quality is established. It is also demonstrated that morphology, crystallinity, wettability and sheet resistance of the VGNs can be varied while maintaining the same sp3 content in the film. The effects of the substrate temperature and the electric field in vertical alignment of the graphene sheets are reported. These findings help to develop and optimize the process conditions to produce VGNs tailored for applications including sensing, field emission, catalysis and energy storage.