Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides

TL;DR

This paper explores how dark excitons influence the optical properties of exciton-polaritons in 2D transition metal dichalcogenides, revealing their role in scattering processes and absorption spectra in the strong-coupling regime.

Contribution

It provides the first detailed analysis of dark exciton signatures in momentum-resolved polariton absorption spectra of hBN-encapsulated WSe₂ and MoSe₂ monolayers.

Findings

Dark excitons significantly affect polariton absorption in WSe₂.

Phonon-mediated scattering leads to step-like features in spectra.

Temperature and mirror reflectance alter polariton optical responses.

Abstract

Integrating 2D materials into high-quality optical microcavities opens the door to fascinating many-particle phenomena including the formation of exciton-polaritons. These are hybrid quasi-particles inheriting properties of both the constituent photons and excitons. In this work, we investigate the so-far overlooked impact of dark excitons on the momentum-resolved absorption spectra of hBN-encapsulated WSe$_2$ and MoSe$_2$ monolayers in the strong-coupling regime. In particular, thanks to the efficient phonon-mediated scattering of polaritons into energetically lower dark exciton states, the absorption of the lower polariton branch in WSe$_2$ is much higher than in MoSe$_2$. It shows unique step-like increases in the momentum-resolved profile indicating opening of specific scattering channels. We study how different externally accessible quantities, such as temperature or mirror reflectance, change the optical response of polaritons. Our study contributes to an improved microscopic understanding of exciton-polaritons and their interaction with phonons, potentially suggesting experiments that could determine the energy of dark exciton states via momentum-resolved polariton absorption.