Raman spectroscopy of graphene under ultrafast laser excitation

C. Ferrante (), A. Virga, L. Benfatto, M. Martinati, D. De Fazio, U. Sassi, C. Fasolato, A. K. Ott, P. Postorino, D. Yoon, G. Cerullo, F. Mauri, A. C. Ferrari and T. Scopigno ()
Additional contact information
C. Ferrante: Universitá di Roma La Sapienza”
A. Virga: Universitá di Roma La Sapienza”
L. Benfatto: CNR, UoS Sapienza
M. Martinati: Universitá di Roma La Sapienza”
D. De Fazio: University of Cambridge
U. Sassi: University of Cambridge
C. Fasolato: Universitá di Roma La Sapienza”
A. K. Ott: University of Cambridge
P. Postorino: Universitá di Roma La Sapienza”
D. Yoon: University of Cambridge
G. Cerullo: Politecnico di Milano
F. Mauri: Universitá di Roma La Sapienza”
A. C. Ferrari: University of Cambridge
T. Scopigno: Universitá di Roma La Sapienza”

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: Abstract The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron–phonon interactions; however, their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3 ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700–3100 K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidths of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones’ broadening and electron–phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics.

Date: 2018
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DOI: 10.1038/s41467-017-02508-x

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