The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellitesʼ photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.
The growing field of quantum information technology requires propagation of information over long distances with efficient readout mechanisms. Excitonic quantum fluids have emerged as a powerful platform for this task due to their straightforward electro-optical conversion. In two-dimensional transition metal dichalcogenides, the coupling between spin and valley provides exciting opportunities for harnessing, manipulating, and storing bits of information. However, the large inhomogeneity of single layers cannot be overcome by the properties of bright excitons, hindering spin-valley transport. Nonetheless, the rich band structure supports dark excitonic states with strong binding energy and longer lifetime, ideally suited for long-range transport. Here we show that dark excitons can diffuse over several micrometers and prove that this repulsion-driven propagation is robust across non-uniform samples. The long-range propagation of dark states with an optical readout mediated by chiral phonons provides a new concept of excitonic devices for applications in both classical and quantum information technology.
more » « less- NSF-PAR ID:
- 10424893
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 14
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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