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

A. Virga, C. Ferrante (), G. Batignani, D. Fazio, A. D. G. Nunn, A. C. Ferrari, G. Cerullo and T. Scopigno ()
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A. Virga: Universitá di Roma
C. Ferrante: Universitá di Roma
G. Batignani: Universitá di Roma
D. Fazio: Cambridge University
A. D. G. Nunn: Istituto Italiano di Tecnologia, Center for Life Nano Science @Sapienza
A. C. Ferrari: Cambridge University
G. Cerullo: IFN-CNR, Dipartimento di Fisica, Politecnico di Milano
T. Scopigno: Universitá di Roma

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11165-1

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