Graphene’s nonlinear-optical physics revealed through exponentially growing self-phase modulation

Nathalie Vermeulen (), David Castelló-Lurbe, Mulham Khoder, Iwona Pasternak, Aleksandra Krajewska, Tymoteusz Ciuk, Wlodek Strupinski, JinLuo Cheng, Hugo Thienpont and Jürgen Erps
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Nathalie Vermeulen: Vrije Universiteit Brussel
David Castelló-Lurbe: Vrije Universiteit Brussel
Mulham Khoder: Vrije Universiteit Brussel
Iwona Pasternak: Institute of Electronic Materials Technology
Aleksandra Krajewska: Institute of Electronic Materials Technology
Tymoteusz Ciuk: Institute of Electronic Materials Technology
Wlodek Strupinski: Warsaw University of Technology
JinLuo Cheng: Chinese Academy of Sciences
Hugo Thienpont: Vrije Universiteit Brussel
Jürgen Erps: Vrije Universiteit Brussel

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Graphene is considered a record-performance nonlinear-optical material on the basis of numerous experiments. The observed strong nonlinear response ascribed to the refractive part of graphene’s electronic third-order susceptibility χ(3) cannot, however, be explained using the relatively modest χ(3) value theoretically predicted for the 2D material. Here we solve this long-standing paradox and demonstrate that, rather than χ(3)-based refraction, a complex phenomenon which we call saturable photoexcited-carrier refraction is at the heart of nonlinear-optical interactions in graphene such as self-phase modulation. Saturable photoexcited-carrier refraction is found to enable self-phase modulation of picosecond optical pulses with exponential-like bandwidth growth along graphene-covered waveguides. Our theory allows explanation of these extraordinary experimental results both qualitatively and quantitatively. It also supports the graphene nonlinearities measured in previous self-phase modulation and self-(de)focusing (Z-scan) experiments. This work signifies a paradigm shift in the understanding of 2D-material nonlinearities and finally enables their full exploitation in next-generation nonlinear-optical devices.

Date: 2018
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DOI: 10.1038/s41467-018-05081-z

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