Intercalation of Few-Layer Graphite Flakes with FeCl3: Raman Determination of Fermi Level, Layer by Layer Decoupling, and Stability

Abstract

We use anhydrous ferric chloride (FeCl₃) to intercalate graphite flakes consisting of 2−4 graphene layers and to dope graphene monolayers. The intercalant, staging, stability, and doping of the resulting intercalation compounds (ICs) are characterized by Raman scattering. The G peak of heavily doped monolayer graphene upshifts to ∼1627 cm⁻¹. The 2−4 layer ICs have similar upshifts, and a Lorentzian line shape for the 2D band, indicating that each layer behaves as a decoupled heavily doped monolayer. By performing Raman measurements at different excitation energies, we show that, for a given doping level, the 2D peak can be suppressed by Pauli blocking for laser energy below the doping level. Thus, multiwavelength Raman spectroscopy allows a direct measurement of the Fermi level, complementary to that derived by performing measurements at fixed excitation energy significantly higher than the doping level. This allows us to estimate a Fermi level shift of up to ∼0.9 eV. These ICs are thus ideal test-beds for the physical and chemical properties of heavily doped graphenes.