Local field effects in ultrafast light-matter interaction measured by pump-probe spectroscopy of monolayer MoSe${}_2$

Abstract

Using a novel approach to ultrafast resonant pump-probe spectroscopy we investigate the spectral shape and dynamics of absorption features related to the A exciton in an hBN/MoSe${}_2$/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 the transition metal dichalcogenide (TMD) system both quantities get thoroughly mixed by strong exciton-exciton interaction. We find that for short positive delays the spectral lines experience pronounced changes in their shape and energy and they relax to the original situation on a picosecond time scale. For negative delays distinctive spectral oscillations appear indicating the first-time observation of perturbed free induction decay for a TMD system. The comparison between co-circular and cross-circular excitation schemes further allows us to investigate the rapid 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 explain all phenomena observed in the experiment with excellent consistency. Our handy model can be even further reduced to two levels in the case of a co-circular excitation, for which we 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 thus fully reproducing the complex behavior of the observed effects.

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Cited by in corpus (5)

• Prolonging Valley Polarization Lifetime through Gate-Controlled Exciton-to-Trion Conversion in Monolayer Molybdenum Ditelluride
• Destructive photon echo formation in six-wave mixing signals of a MoSe${}_2$ monolayer
• Fundamentals of heterodyne wave mixing spectroscopy: a tutorial
• Photoluminescence efficiency of MBE-grown MoSe${}_2$ monolayers featuring sharp excitonic lines and diverse grain structures
• Uniform Narrow Excitonic Spectrum in Large-Area Suspended WSe2 Monolayers