Multi-dimensional spectroscopy of mobile excitons in two-dimensional semiconductors

Abstract: Multi-dimensional coherent spectroscopy (MDCS) goes beyond standard linear-response probes and provides a powerful tool for investigating correlations between quasiparticles such as excitons (bound electron-hole pairs). Here we present a microscopic theory of MDCS that accounts for the delocalized nature of excitons in two-dimensional semiconductors. In contrast to the more phenomenological few-level approaches typically employed for modelling MDCS, our theory features mobile excitons with continuous momentum degrees of freedom. We find that the energy continuum associated with exciton momenta is crucial for producing interaction-induced decoherence, as well as capturing the interference between different exciton-polaron quasiparticles in the case of charge-doped semiconductors. Crucially, our calculated MDCS spectra agree well with recent experiments on doped monolayer MoSe$_2$ [Hao et al., Nature Communications 8, 15552 (2017)], and they suggest that the interactions between exciton polarons depend strongly on phase-space filling effects, where exciton polarons compete for electrons. Our results demonstrate that microscopic approaches allow one to gain new insights from the fine structure of MDCS on two-dimensional semiconductors, and they illustrate the utility of microscopic approaches to modelling MDCS experiments more generally.