Highly Decoupled Graphene Multilayers: Turbostraticity at its Best

The extraordinary properties of graphene are truly observable when it is suspended, being free from any substrate influence. Here, a new type of multilayer graphene is reported wherein each layer is turbostratically decoupled, resembling suspended graphene in nature, while maintaining high degree of 2D crystallinity. Such defect-free graphene multilayers have been made over large areas by Joule heating of a Ni foil coated with a solid hydrocarbon. Raman spectra measured on thick flakes of turbostratically single layer graphene (T-SLG) (100-250 nm) have shown characteristics similar to suspended graphene with very narrow 2D bands (∼16 cm(-1)) and I2D/IG ratios up to 7.4, importantly with no D band intensity. Electron diffraction patterns showed sets of diffraction spots spread out with definite angular spacings, reminiscent of the angular deviations from the AB packing which are responsible for keeping the layers decoupled. The d-spacing derived from X-ray diffraction was larger (by ∼0.04 Å) compared to that in graphite. Accordingly, the c-axis resistance values were three orders higher, suggesting that the layers are indeed electronically decoupled. The high 2D crystallinity observed along with the decoupled nature should accredit the observed graphene species as a close cousin of suspended graphene.