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Generally, the broadening of the D peak is correlated to a distribution of sp2 clusters with different orders and dimensions, and the width of the G peak is proportional to the bond-angle disorder at sp2 sites, that is, both D and G peaks FWHM broaden due to disorder (Phys. Rev. B, 2000, 61, 14095; Solid State Commun., 2007, 143, 47). During the GQDs preparation, a large amount of surface defects including carbonyl, carboxyl, hydroxyl, and epoxy groups were introduced to the edges and onto the basal plane, and more hydroxyl defects are formed in rGQDs. Thus, it is the increase of disorders in GQDs that lead to the broadening of D and G peaks. These results also agree with HR-TEM observation, in which the short range order and a loss of long distance translational periodicity is always found. On the other hand, this particular broadening in the Raman bands could be due to the relaxation of the double-resonance Raman selection rules associated with the random orientation of GQDs with respect to each other (Appl. Phys. Lett., 2013, 102, 53108).
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