Microscopic many-body theory of two-dimensional coherent spectroscopy of excitons and trions in atomically thin transition metal dichalcogenides

Abstract: We present a microscopic many-body theory of the recently measured two-dimensional coherent spectroscopy (2DCS) of excitons and trions in monolayer MoSe$_{2}$ materials {[}K. Hao \textit{et al.}, Nano Lett. \textbf{16}, 5109 (2016){]}, where excitons and trions can be well interpreted as repulsive and attractive polarons, respectively, in the dilute limit of exciton density. We derive a simple relation for the 2DCS spectrum in terms of a modified, mixing time-dependent polaron Green function, which is valid in the single exciton limit. Our simulated spectra are in excellent qualitative agreement with experiments without introducing any phenomenological parameters such as decoherence rates. In particular, quantum beats between the off-diagonal crosspeaks in the experimental 2DCS spectra are well reproduced. Our work, therefore, clarifies the microscopic principle that underlies the observed optical signals of exciton-trion coherence. We find that there are two quantitative discrepancies between theory and experiment: the smaller than expected crosspeak strength and the slightly unsynchronized quantum beats at different crosspeaks. Tentatively, we attribute these residual discrepancies to the finite exciton density and the resultant polaron-polaron interaction, which is not taken into account in our theory.