Radiatively Limited Dephasing and Exciton Dynamics in MoSe ₂ Monolayers Revealed with Four-Wave Mixing Microscopy

Abstract

By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe ₂. We reveal their dephasing times T ₂ and radiative lifetime T ₁ in a subpicosecond (ps) range, approaching T ₂ = 2 T ₁ and thus indicating radiatively limited dephasing at a temperature of 6 K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder. At the nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse toward the dark states but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer intervalley exciton dynamics, revealing an initial polarization degree of around 30%, constant during the initial subpicosecond decay, followed by the depolarization on a picosecond time scale. The FWM hyperspectral imaging reveals the doped and undoped areas of the sample, allowing us to investigate the neutral exciton, the charged one, or both transitions at the same time. In the latter, we observe the exciton–trion beating in the coherence evolution indicating their coherent coupling.