By means of the ultrafast optical Kerr effect method coupled to optical heterodyne detection (OHD-OKE), we characterize the third-order nonlinear response of graphene and compare it to experimental values obtained by the Z-scan method on the same samples. From these measurements, we estimate a negative nonlinear refractive index for monolayer graphene, n2=-1.1×10-13 m2/W. This is in contradiction to previously reported values, which leads us to compare our experimental measurements obtained by the OHD-OKE and the Z-scan method with theoretical and experimental values found in the literature and to discuss the discrepancies, taking into account parameters such as doping.
Using an enhanced optically heterodyned optical Kerr effect method and a theoretical description of the interactions between an optical beam, a single layer of graphene, and its substrate, we provide experimental answers to questions raised by theoretical models of graphene third-order nonlinear optical response. In particular, we measure separately the time response of the two main tensor components of the nonlinear susceptibility, we validate the assumption that the out-of plane tensor components are small, and we quantify the optical impact of the substrate on the measured coefficients. Our method can be applied to other 2D materials, as it relies mainly on the small ratio between the thickness and the wavelength.
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