Near-Unity Light Absorption in a Monolayer WS2 Van der Waals Heterostructure Cavity

Nano Lett. 2020 May 13;20(5):3545-3552. doi: 10.1021/acs.nanolett.0c00492. Epub 2020 Apr 20.

Abstract

Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultralow excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light-exciton-cavity interaction. We find that the subtle interplay between the radiative, nonradiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light-exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.

Keywords: 2D materials; Exciton complexes; Light-matter interaction; TMD Excitons; Unity absorption.