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 nonequilibrium temperatures in the similar to 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.
Raman spectroscopy of graphene under ultrafast laser excitation / Ferrante, C.; Virga, A.; Benfatto, L.; Martinati, M.; De Fazio, D.; Sassi, U.; Fasolato, C.; Ott, A. K.; Postorino, P.; Yoon, D.; Cerullo, G.; Mauri, F.; Ferrari, A. C.; Scopigno, T.. - In: NATURE COMMUNICATIONS. - ISSN 2041-1723. - 9:(2018). [10.1038/s41467-017-02508-x]
Raman spectroscopy of graphene under ultrafast laser excitation
Ferrante, C.;Fasolato, C.;Postorino, P.;Mauri, F.;Scopigno, T.
2018
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 nonequilibrium temperatures in the similar to 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.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
