Local field effects in ultrafast light-matter interaction measured by pump-probe spectroscopy of monolayer MoSe$_{\boldsymbol 2}$

TL;DR

This study employs a novel ultrafast pump-probe spectroscopy technique to explore local field effects and exciton dynamics in monolayer MoSe₂, revealing complex spectral behaviors and inter-valley scattering phenomena.

Contribution

It introduces a three-level model incorporating local field effects, excitation dephasing, and scattering to explain complex ultrafast spectral dynamics in TMD monolayers.

Findings

Observation of spectral shape and energy changes on picosecond timescales.

First-time detection of perturbed free induction decay in TMDs.

Analytic solutions for co-circular excitation revealing local field and dephasing impacts.

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.