Optical Third-Harmonic Generation in Graphene

We report strong third-harmonic generation (THG) in monolayer graphene grown by chemical vapor deposition (CVD) and transferred to an amorphous silica (glass) substrate; the photon energy is in three-photon resonance with the exciton-shifted van Hove singularity at the M-point of graphene. Our polarization- and azimuthal-rotation-dependent measurements confirm the expected symmetry properties for this nonlinear process. Since the third-harmonic signal exceeds that of bulk glass by more than two orders of magnitude, the signal contrast permits background-free scanning of graphene and provides insight into the structural properties of graphene.