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

Accepted version
Peer-reviewed

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Authors

Virga, A 
De Fazio, D 
Nunn, ADG 

Abstract

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.

Description

Keywords

cond-mat.mes-hall, cond-mat.mes-hall, physics.optics

Journal Title

Nat Commun

Conference Name

Journal ISSN

2041-1723
2041-1723

Volume Title

10

Publisher

Springer Science and Business Media LLC

Rights

All rights reserved
Sponsorship
Royal Society (JP080053)
Engineering and Physical Sciences Research Council (EP/K01711X/1)
Engineering and Physical Sciences Research Council (EP/K017144/1)
European Commission (604391)
Engineering and Physical Sciences Research Council (EP/L016087/1)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (696656)
EPSRC (via University of Manchester) (R119256)
European Commission Horizon 2020 (H2020) Societal Challenges (732344)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (785219)
Engineering and Physical Sciences Research Council (EP/G042357/1)
The Royal Society (uf072943)
Royal Society (516002K5698/kk)
European Research Council (319277)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (820378)
European Research Council (842251)