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We report the growth of thickness-controlled rotationally faulted multilayergraphene (rf-MLG) on Ni foils by low-pressure chemical vapor deposition andtheir characterization by micro-Raman spectroscopy. The surface morphology andthickness were investigated by scanning electron microscope, X-ray diffraction,and transmittance measurements. These results have revealed that the thicknessof rf-MLG can be effectively controlled by the thickness of the Ni foil ratherthan the flow rate of CH$_4$, H$_2$, Ar. In the Raman spectroscopymeasurements, we observed most Raman peaks of the graphitic materials. Ramanspectra can be categorized into four patterns and show systematic behaviors.Especially, the in-plane (~1880 cm$^{-1}$, ~2035 cm$^{-1}$) and out-of-plane(~1750 cm$^{-1}$) modes are successfully analyzed to explain the dimensionalityof rf-MLG as in the twisted (or rotated) bilayer graphene. In addition, it isfound that the two peaks at ~1230 cm$^{-1}$ and ~2220 cm$^{-1}$ well reflectthe properties of the in-plane mode. The peak intensities of the above fourin-plane modes are proportional to that of 2D band, indicating that they sharethe common Raman resonance process.

Growth and Raman spectroscopy of thickness-controlled rotationally faulted multilayer graphene