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The shape of coherent anti-Stokes Raman scattering (CARS) spectral line depends on the ratio of the vibrational and electronic contributions to the third-order susceptibility of the material. The G-mode (1590 cm −1 ) of graphene and carbon nanotubes (CNTs) exhibits opposite features in the CARS spectrum, showing “dip” and “peak,” respectively. Here, we consider the CARS spectra of graphene and carbon nanotubes in terms of Fano formalism describing the line shapes of CARS resonances. We show that imaging at only 1590 cm −1  is not sufficient to separate the constituents of a composite material consisting of both graphene and CNTs. We propose an algorithm to map the graphene and CNTs in a composite material.

Recognition of Spatial Distribution of CNT and Graphene in Hybrid Structure by Mapping with Coherent Anti-Stokes Raman Microscopy