Effect of pressure and hydrogen flow in nucleation density and morphology of graphene bidimensional crystals

In this paper we present new results concerning the growth of graphene by low pressure chemical vapor deposition on polycrystalline copper foils and using methane as carbon precursor. We have studied the role of hydrogen and pressure in graphene growth on substrates of polycrystalline copper foil and we have examined how they affect the nucleation density and the size of graphene bidimensional crystals. For that, small ranges of pressure (between 10 and 30 Pa) and hydrogen flow (between 10 and 20 sccm) were explored. In addition, the antagonism between two of the main effects of hydrogen was studied. Hydrogen promotes the growth but, at the same time, applies an intense dry etching during the growth process of graphene. The challenge of the present study is to find the equilibrium between these two effects so that, the growth of highly ordered crystals on copper becomes possible. The results reveal that the total pressure during the growth process of graphene affects the size as well as the nucleation density of the graphene bidimensional crystals on polycrystalline copper. Besides, the hydrogen flow affects the morphology and quality of the graphene layer. An important parameter for a correct interpretation of the results is the change of the partial pressure ratio, , during the growth process under a constant flow of H2 and CH4. Dendritic graphene crystals with lobe lengths around 30 μm along with a nucleation density of 25 nuclei/10 000 μm2 were obtained in the studied technological conditions, which corroborates that a low nucleation of graphene is required to obtain large graphene islands and a low number of crystal boundaries. Raman spectroscopy and scanning electron microscopy evidenced the effects of hydrogen on the characteristics of growth and morphology of the graphene dendritic bidimensional crystals.