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The equilibrium optical phonons of graphene are well characterized in termsof anharmonicity and electron-phonon interactions, however theirnon-equilibrium properties in the presence of hot charge carriers are still notfully explored. Here we study the Raman spectrum of graphene under ultrafastlaser excitation with 3ps pulses, which trade off between impulsive stimulationand spectral resolution. We localize energy into hot carriers, generatingnon-equilibrium temperatures in the ~1700-3100K range, far exceeding that ofthe phonon bath, while simultaneously detecting the Raman response. Thelinewidth of both G and 2D peaks show an increase as function of the electronictemperature. We explain this as a result of the Dirac cones' broadening andelectron-phonon scattering in the highly excited transient regime, importantfor the emerging field of graphene-based photonics and optoelectronics.

Raman spectroscopy of graphene under ultrafast laser excitation