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Raman spectroscopy is a powerful approach to investigating the structural and electronic properties of carbon-based materials. The shape of the second-order Raman band (2D) is a characteristic that can be used to distinguish the number of layers of AB-stacked grapheme 24¨C26. We carried out confocal Raman mapping on single-, biand trilayer GNRs (Methods). We obtained an AFM image (Fig. 3a) and a G-band image (Fig. 3b) of a 0.9-nm-thick GNR on the same length scale. The 2D peak was well fitted by a sharp and symmetric Lorentzian peak (inset, Fig. 3c), suggesting the single-layer nature of the GNR. For another 1.3-nm-thick GNR (Fig. 3d¨Cf), the 2D peak was fitted by four Lorentzians (inset, Fig. 3f), characteristic of bilayer,AB-stacked graphene. Some bilayer GNRs showed 2D peaks with different line shapes from AB-stacked graphene, reflecting the varying stacking structures between layers in the starting MWCNTs (Supplementary Fig. 2). For a trilayer GNR (height, ,1.9 nm; see Supplementary Fig. 3), similar to trilayer, ABA-stacked grapheme sheets, the 2D band was broader and up shifted as the thickness increased (Supplementary Table 1). We note that the 2D band of the MWCNTs was broader than that of our GNRs (Supplementary Fig. 6), as expected.

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