Nano Letters · 2020 · 94 citations · 60 references
Natural SciencesMaterials SciencePhysicsCondensed Matter PhysicsOptical MaterialsPhotonicsOptical Properties Of SemiconductorsOptical Properties Of SolidsQuantum OptoelectronicsSemiconductor NanomaterialsTwo-dimensional NanomaterialsTwo-dimensional SemiconductorsDecay RatesExcitonsLight AbsorptionLight-matter InteractionNonlinear Optical ResponseStrong Light-matter CouplingTransition Metal DichalcogenidesVan Der Waals Heterostructures
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.
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