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Second-order Overtone and Combinational Raman Modes of Graphene Layers in the Range of 1690 cm-1 to 2150 cm-1

Though graphene has been intensively studied by Raman spectroscopy, in this letter, we report a study of second-order overtone and combinational Raman modes in an unexplored range of 1690-2150 cm-1 in nonsuspended commensurate (AB-stacked), incommensurate (folded) and suspended graphene layers. Based on the double resonance theory, four dominant modes in this range have been assigned as 2oTO (M band), iTA+LO, iTO+LA and LO+LA. Differing to AB-stacked bilayer graphene or few layer graphene, the M band disappears in single layer graphene. Systematic analysis reveals that interlayer interaction is essential for the presence (or absence) of M band whereas the substrate has no effect on this. Dispersive behaviors of these "new" Raman modes in graphene have been probed by the excitation energy dependent Raman spectroscopy. It is found that the appearance of the M band strictly relies on the AB stacking, which could be a fingerprint of AB-stacked bilayer graphene. This work expands the unique and powerful abilities of Raman spectroscopy on study of graphene and provides another effective way to probe phonon dispersion, electron-phonon coupling, and to exploit electronic band structure of graphene layers.