*Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies have addressed the general operation of graphene-based photothermoelectric devices and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster timescale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 fs. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 fs laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity of between 500 and 1,500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.
Photovoltage generation through the photothermoelectric (PTE) effect occurs when light is focused at the interface of monolayer and bilayer graphene, or at the interface between regions of graphene with different Fermi energies E F (refs 1-6). In such graphene PTE devices-which operate over a large spectral range 7,8 that extends even into the far-infrared 9 -local heating of electrons by absorbed light, in combination with a difference in Seebeck coefficients between the two regions, gives rise to a PTE voltage V PTE = (S 2 − S 1 )(T el − T 0 ). Here, S 1 and S 2 are the Seebeck coefficients of regions 1 and 2, respectively, T el is the hot electron temperature after photoexcitation and electron heating, and T 0 is the temperature of the electrode heat sinks. The performance of PTE graphene devices is intimately connected to the dynamics of the photoexcited electrons and holes, which have mainly been studied in graphene samples through ultrafast optical pumpprobe measurements [10][11][12][13][14][15][16][17] . As shown in Fig. 1a, the dynamics start with (i) photoexcitation and electron-hole pair generation, followed by (ii) electron heating through carrier-carrier scattering, in competition with lattice heating, both of which take place on a sub-100 fs timescale, and finally (iii) electron cooling by thermal equilibration with the lattice, which takes place on a picosecond timescale. The effect of the picosecond cooling step (iii) on the switching speed of graphene devices has been studied using timeresolved photovoltage scanning experiments with ∼200 fs time resolution [18][19][20] . These studies showed that the picosecond electron cooling time limits the intrinsic photo-switching rate of these devices to a few hundred gigahertz, because faster switching would reduce the switching contrast, as the system does not have time to return to the ground state. Indeed, gigahertz switching speeds have been demonstrated in graphene-based devices [21][22][23]...