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Third-order optical nonlinearities of graphene from monolayer to multilayers were investigated in the femtosecond regime, and the contribution of interlayer coupling to the nonlinearities was studied. The nonlinear refractive index γ of the order of 10−9 cm2/W and the nonlinear absorption coefficient β of 10−6 cm/W were obtained. By systematically investigating the nonlinear optical properties with the number of layers and comparing the coupling graphene with the decoupling superimposed graphene, we found that the coupling of interlayers has large effect upon the nonlinear refraction. These results provide an effective approach for developing graphene-based nonlinear photonic devices

The nonlinear optical properties of coupling and decoupling graphene layers