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

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 et al. [Nat. Phys. 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.