Raman identification of edge alignment of bilayer graphene down to the nanometer scale

The ideal edges of bilayer graphene (BLG) are that the edges of the top and bottom graphene layers (GLs) of BLG are well-aligned. Actually, the alignment distance between the edges of the top and bottom GLs of a real BLG can be as large as the submicrometer scale or as small as zero, which cannot be distinguished using an optical microscope. Here, we present a detailed Raman study on BLG at its edges. If the alignment distance of the top and bottom GLs of BLG is larger than the laser spot, the measured D mode at the edge of the top GL of BLG shows a similar spectral profile to that of disordered BLG. If the alignment distance is smaller than the laser spot, the D mode at a real BLG edge shows three typical spectral profiles similar to that at the edge of SLG, that of the well-aligned edge of BLG, or a combination of both. We show the sensitivity and ability of Raman spectroscopy to acquire the alignment distance between two edges of top and bottom GLs of BLG as small as several nanometers, which is far beyond the diffraction limit of a laser spot. This work opens the possibility to probe the edge alignment of multi-layer graphene.