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

Nathalie Vermeulen¹, David Castelló-Lurbe^2,3, Mulham Khoder²

¹Brussels Photonics, Dept. of Applied Physics and Photonics, Vrije Universiteit Brussel, Pleinlaan 2, 1050, Brussel, Belgium. nvermeul@b-phot.org.

Nature Communications

|July 12, 2018

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Researchers solved the paradox of graphene's strong nonlinear-optical effects. A new phenomenon, saturable photoexcited-carrier refraction, explains graphene's performance, enabling advanced nonlinear-optical devices.

Area of Science:

Nonlinear Optics
Materials Science
Condensed Matter Physics

Background:

Graphene exhibits exceptional nonlinear-optical properties, surpassing theoretical predictions.
The strong nonlinear response was previously attributed to third-order susceptibility (χ(3)), but this did not align with experimental observations.

Purpose of the Study:

To resolve the discrepancy between theoretical predictions and experimental results for graphene's nonlinear-optical behavior.
To identify and characterize the underlying mechanism responsible for graphene's strong nonlinear optical effects.

Main Methods:

Theoretical modeling of nonlinear-optical interactions in graphene.
Experimental validation using graphene-covered waveguides and picosecond optical pulses.
Analysis of self-phase modulation and self-(de)focusing (Z-scan) experiments.

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Main Results:

Demonstrated that saturable photoexcited-carrier refraction, not χ(3)-based refraction, dominates graphene's nonlinear-optical interactions.
Observed exponential-like bandwidth growth in self-phase modulation of picosecond pulses in graphene waveguides.
Validated the new theoretical framework against existing experimental data for self-phase modulation and Z-scan measurements.

Conclusions:

Introduced a new understanding of nonlinearities in two-dimensional (2D) materials, shifting the paradigm from χ(3) to saturable photoexcited-carrier refraction.
The findings quantitatively explain previously paradoxical experimental results in graphene.
This research paves the way for the optimized design and application of graphene in next-generation nonlinear-optical devices.