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Near-unity light absorption in a monolayer WS2 van der Waals heterostructure cavity

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 Added by Itai Epstein
 Publication date 2019
  fields Physics
and research's language is English




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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 ultra-low 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, non-radiative 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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The atomic-level vdW heterostructures have been one of the most interesting quantum material systems, due to their exotic physical properties. The interlayer coupling in these systems plays a critical role to realize novel physical observation and enrich interface functionality. However, there is still lack of investigation on the tuning of interlayer coupling in a quantitative way. A prospective strategy to tune the interlayer coupling is to change the electronic structure and interlayer distance by high pressure, which is a well-established method to tune the physical properties. Here, we construct a high-quality WS2/MoSe2 heterostructure in a DAC and successfully tuned the interlayer coupling through hydrostatic pressure. Typical photoluminescence spectra of the monolayer MoSe2 (ML-MoSe2), monolayer WS2 (ML-WS2) and WS2/MoSe2 heterostructure have been observed and its intriguing that their photoluminescence peaks shift with respect to applied pressure in a quite different way. The intralayer exciton of ML-MoSe2 and ML-WS2 show blue shift under high pressure with a coefficient of 19.8 meV/GPa and 9.3 meV/GPa, respectively, while their interlayer exciton shows relative weak pressure dependence with a coefficient of 3.4 meV/GPa. Meanwhile, external pressure helps to drive stronger interlayer interaction and results in a higher ratio of interlayer/intralayer exciton intensity, indicating the enhanced interlayer exciton behavior. The first-principles calculation reveals the stronger interlayer interaction which leads to enhanced interlayer exciton behavior in WS2/MoSe2 heterostructure under external pressure and reveals the robust peak of interlayer exciton. This work provides an effective strategy to study the interlayer interaction in vdW heterostructures, which could be of great importance for the material and device design in various similar quantum systems.
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