Two-dimensional coherent spectroscopy of trion-polaritons and exciton-polaritons in atomically thin transition metal dichalcogenides

TL;DR

This paper provides a microscopic theoretical analysis of two-dimensional coherent spectroscopy of trion-polaritons and exciton-polaritons in monolayer transition metal dichalcogenides, revealing detailed quasiparticle interactions and spectral features.

Contribution

It introduces a microscopic many-body calculation method for 2DCS of trion- and exciton-polaritons, including the effects of charge tunability and quasiparticle residues.

Findings

Prediction of three off-diagonal cross-peaks indicating coherence among polariton branches.

Confirmation that light-matter coupling depends on trion quasiparticle residue.

Microscopic calculation of nonlinear 2DCS spectrum for both trion- and exciton-polaritons.

Abstract

We present a microscopic many-body calculation of the nonlinear two-dimensional coherent spectroscopy (2DCS) of trion-polaritons and exciton-polaritons in charge-tunable transition-metal-dichalcogenides monolayers placed in an optical microcavity. The charge tunability leads to an electron gas with nonzero density that brings brightness to the trion - a polaron quasiparticle formed by an exciton with a nonzero residue bounded to the electron gas. As a result, a trion-polariton is created under strong light-matter coupling, as observed in the recent experiment by Sidler \textit{et al.} {[}Nat. Phys. \textbf{13}, 255 (2017){]}. We analyze in detail the structure of trion-polaritons, by solving an extended Chevy ansatz for the trion quasiparticle wave-function. We confirm that the effective light-matter coupling for trion-polaritons is determined by the residue of the trion quasiparticle. The solution of the full many-body polaron states within Chevy ansatz enables us to microscopically calculate the nonlinear 2DCS spectrum of both trion-polaritons and exciton-polaritons. We predict the existence of three kinds of off-diagonal cross-peaks in the 2DCS spectrum, as an indication of the coherence among the different branches of trion-polaritons and exciton-polaritons. Due to the sensitivity of 2DCS spectrum to quasiparticle interactions, our work provides a good starting point to explore the strong nonlinearity exhibited by trion-polaritons in some recent exciton-polariton experiments.