Exciton dynamics in hBN/MoSe2/hBN heterostructures measured in pump-probe spectroscopy

Using ultrafast resonant pump-probe spectroscopy we investigate A exciton dynamics in an hBN/MoSe2/hBN van der Waals heterostructure. While in a pure two-level system a pump-probe experiment measures the occupation or the polarization dynamics, depending on the time ordering of the pulse pair, in our case both quantities get mixed by the interaction of the excitons. We find that for short positive delays the spectral lines are blue-shifted and that they relax to the original energy on a picosecond time scale. For negative delays pronounced spectral oscillations appear. The comparison between co-circular and cross-circular excitation schemes further allows us to investigate the inter-valley scattering. By considering a three-level system as a minimal model including the local field effect, excitation induced dephasing and scattering between the excited states we can explain all phenomena observed in the experiment. Our model can be reduced to two levels in the case of a co-circular excitation, for which we can derive analytic expressions to describe the detected signals. This allows us to trace back the spectral shapes and shifts to the impact of local field effect and excitation induced dephasing.