Atomically thin, two-dimensional, transition-metal dichalcogenide (TMD) monolayers have recently emerged as a versatile platform for optoelectronics. Their appeal stems from a tunable direct bandgap in the visible and near-infrared regions, the ability to enable strong coupling to light, and the unique opportunity to address the valley degree of freedom over atomically thin layers. Additionally, monolayer TMDs can host defect-bound localized excitons that behave as single-photon emitters, opening exciting avenues for highly integrated 2D quantum photonic circuitry. By introducing plasmonic nanostructures and metasurfaces, one may effectively enhance light harvesting, direct valley-polarized emission, and route valley index. This review article focuses on these critical aspects to develop integrated photonic and valleytronic applications by exploiting exciton–plasmon coupling over a new hybrid material platform.
As hosts for tightly-bound electron-hole pairs carrying quantized angular momentum, atomically-thin semiconductors of transition metal dichalcogenides (TMDCs) provide an appealing platform for optically addressing the valley degree of freedom. In particular, the valleytronic properties of neutral and charged excitons in these systems have been widely investigated. Meanwhile, correlated quantum states involving more particles are still elusive and controversial despite recent efforts. Here, we present experimental evidence for four-particle biexcitons and five-particle exciton-trions in high-quality monolayer tungsten diselenide. Through charge doping, thermal activation, and magnetic-field tuning measurements, we determine that the biexciton and the exciton-trion are bound with respect to the bright exciton and the trion, respectively. Further, both the biexciton and the exciton-trion are intervalley complexes involving dark excitons, giving rise to emissions with large, negative valley polarization in contrast to that of the two-particle excitons. Our studies provide opportunities for building valleytronic quantum devices harnessing high-order TMDC excitations.
more » « less- NSF-PAR ID:
- 10154320
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 9
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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