Terahertz Generation by Dynamical Photon Drag Effect in Graphene Excited by Femtosecond Optical Pulses

Graphene has been proposed as a particularly attractive material for the achievement of strong optical nonlinearities, in particular generation of terahertz radiation. However, owing to the particular symmetries of the C-lattice, second-order nonlinear effects such as difference-frequency or rectification processes are predicted to vanish in a graphene layer for optical excitations (ℏω ≫ 2EF) involving the two relativistic dispersion bands. Here we experimentally demonstrate that graphene excited by femtosecond optical pulses generate a coherent THz radiation ranging from 0.1 to 4 THz via a second-order nonlinear effect. We fully interpret its characteristics with a model describing the electron and hole states beyond the usual massless relativistic scheme. This second-order nonlinear effect is dynamical photon drag, which relies on the transfer of light momentum to the carriers by the ponderomotive electric and magnetic forces. The model highlights the key roles of next-C-neighbor couplings and of unequal electron and hole lifetimes in the observed second-order response. Finally, our results indicate that dynamical photon drag effect in graphene can provide emission up to 60 THz, opening new routes for the generation of ultrabroadband terahertz pulses.