Coherent anti-Stokes Raman spectroscopy of single and multi-layer graphene

Spontaneous Raman spectroscopy is a powerful characterization tool for graphene research. Its extension to the coherent regime, despite the large nonlinear third-order susceptibility of graphene, has so far proven challenging. Due to its gapless nature, several interfering electronic and phononic tr...

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Bibliographic Details
Published in:Nature communications 2019-08, Vol.10 (1), p.3658-9, Article 3658
Main Authors: Virga, A., Ferrante, C., Batignani, G., De Fazio, D., Nunn, A. D. G., Ferrari, A. C., Cerullo, G., Scopigno, T.
Format: Article
Language:English
Subjects:
140/133
639/301/357/918/1054
639/624/1107/527/1821
639/624/400/385
Coherent scattering
Graphene
Humanities and Social Sciences
multidisciplinary
Multilayers
Raman spectra
Raman spectroscopy
Scatter diagrams
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
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Summary:Spontaneous Raman spectroscopy is a powerful characterization tool for graphene research. Its extension to the coherent regime, despite the large nonlinear third-order susceptibility of graphene, has so far proven challenging. Due to its gapless nature, several interfering electronic and phononic transitions concur to generate its optical response, preventing to retrieve spectral profiles analogous to those of spontaneous Raman. Here we report stimulated Raman spectroscopy of the G-phonon in single and multi-layer graphene, through coherent anti-Stokes Raman Scattering. The nonlinear signal is dominated by a vibrationally non-resonant background, obscuring the Raman lineshape. We demonstrate that the vibrationally resonant coherent anti-Stokes Raman Scattering peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the vibrationally non-resonant background. We model the spectra, taking into account the electronically resonant nature of both. We show how coherent anti-Stokes Raman Scattering can be used for graphene imaging with vibrational sensitivity. Coherent anti-Stokes Raman Scattering (CARS) accesses the vibrational properties of a material via nonlinear four-wave mixing (FWM); CARS in graphene has not been observed to date despite its high nonlinear third-order susceptibility. Here, the authors devised a FWM scheme to perform stimulated Raman spectroscopy in single and multi-layer graphene through CARS.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-11165-1