Graphene with massless Dirac fermions can have exceptionally strong third-order optical nonlinearities. Yet reported values of nonlinear optical susceptibilities for third-harmonic generation (THG), four-wave mixing (FWM) and self-phase modulation vary over six orders of magnitude. Such variation likely arises from frequency-dependent resonance effects of different processes in graphene under different doping. Here, we report an experimental study of THG and FWM in graphene using gate tuning to adjust the doping level and vary the resonant condition. We find that THG and sum-frequency FWM are strongly enhanced in heavily doped graphene, while the difference-frequency FWM appears just the opposite. Difference-frequency FWM exhibited a novel divergence towards the degenerate case in undoped graphene, leading to a giant enhancement of the nonlinearity. The results are well supported by theory. Our full understanding of the diverse nonlinearity of graphene paves the way towards future design of graphene-based nonlinear optoelectronic devices.
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The work at Fudan University was supported by the National Basic Research Program of China (grant no. 2014CB921601), National Key Research and Development Program of China (grant nos. 2016YFA0301002, 2016YFA0300900), National Natural Science Foundation of China (grant no. 91421108, 11622429, 11374065), and the Science and Technology Commission of Shanghai Municipality (grant no. 16JC1400401). Part of the sample fabrication was performed at Fudan Nano-fabrication Laboratory. K.L. is supported by the National Natural Science Foundation of China (grant no. 51522201). J.E.S. is supported by the Natural Sciences and Engineering Research Council of Canada. Y.-R.S. acknowledges support from the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, US Department of Energy (contract no. DE-AC03-76SF00098).
The authors declare no competing interests.
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Jiang, T., Huang, D., Cheng, J. et al. Gate-tunable third-order nonlinear optical response of massless Dirac fermions in graphene. Nature Photon 12, 430–436 (2018). https://doi.org/10.1038/s41566-018-0175-7
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