  The two-dimensional semiconductor MoS2 in its mono- and few-layer form is
expected to have a significant exciton binding energy of several 100 meV,
leading to the consensus that excitons are the primary photoexcited species.
Nevertheless, even single layers show a strong photovoltaic effect and work as
the active material in high sensitivity photodetectors, thus indicating
efficient charge carrier photogeneration (CPG). Here we use continuous wave
photomodulation spectroscopy to identify the optical signature of long-lived
charge carriers and femtosecond pump-probe spectroscopy to follow the CPG
dynamics. We find that intitial photoexcitation yields a branching between
excitons and charge carriers, followed by excitation energy dependent hot
exciton dissociation as an additional CPG mechanism. Based on these findings,
we make simple suggestions for the design of more efficient MoS2 photovoltaic
and photodetector devices.
