Elucidating layer-resolved charge distribution in van der Waals stacked crystals is crucial for electronic applications based on 2D materials. Here, we use CVD-grown few-layer graphene (FLG) labeled by carbon isotopes as a prototype, in which Raman features of two isotope components identify distinct layers. Electrical transfer characteristics of graphene field-effect transistors (GFETs) are employed to quantitatively calibrate the correspondence of Fermi level and G-phonon frequency that shifts with the charge-carrier concentration (n) variation. The isotope-assisted spectroscopy reveals previously unprobed characteristics that the n value of both top and bottom layers in FLG is close rather than following an exponential decay law. This negligible gradient likely benefits from the π−π interaction that favors the interlayer diffusion of charges. In addition, each extra layer reduces the degree of charge exchange at the graphene/dopant interface. These results have important implications for FLG nanoelectronics and provide a robust framework by which one can further investigate the critical properties of other 2D systems.
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