Two-dimensional (2D) materials have attracted attention for quantum information science due to their ability to host single-photon emitters (SPEs). Although the properties of atomically thin materials are highly sensitive to surface modification, chemical functionalization remains unexplored in the design and control of 2D material SPEs. Here, we report a chemomechanical approach to modify SPEs in monolayer WSe2through the synergistic combination of localized mechanical strain and noncovalent surface functionalization with aryl diazonium chemistry. Following the deposition of an aryl oligomer adlayer, the spectrally complex defect-related emission of strained monolayer WSe2is simplified into spectrally isolated SPEs with high single-photon purity. Density functional theory calculations reveal energetic alignment between WSe2defect states and adsorbed aryl oligomer energy levels, thus providing insight into the observed chemomechanically modified quantum emission. By revealing conditions under which chemical functionalization tunes SPEs, this work broadens the parameter space for controlling quantum emission in 2D materials.
Solid‐state single photon emitters (SPEs) within atomically thin transition metal dichalcogenides (TMDs) have recently attracted interest as scalable quantum light sources for quantum photonic technologies. Among TMDs, WSe2monolayers (MLs) are promising for the deterministic fabrication and engineering of SPEs using local strain fields. The ability to reliably produce isolatable SPEs in WSe2is currently impeded by the presence of numerous spectrally overlapping states that occur at strained locations. Here nanoparticle (NP) arrays with precisely defined positions and sizes are employed to deterministically create strain fields in WSe2MLs, thus enabling the systematic investigation and control of SPE formation. Using this platform, electron beam irradiation at NP‐strained locations transforms spectrally overlapped sub‐bandgap emission states into isolatable, anti‐bunched quantum emitters. The dependence of the emission spectra of WSe2MLs as a function of strain magnitude and exposure time to electron beam irradiation is quantified and provides insight into the mechanism for SPE production. Excitons selectively funnel through strongly coupled sub‐bandgap states introduced by electron beam irradiation, which suppresses spectrally overlapping emission pathways and leads to measurable anti‐bunched behavior. The findings provide a strategy to generate isolatable SPEs in 2D materials with a well‐defined energy range.more » « less
- NSF-PAR ID:
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Medium: X
- Sponsoring Org:
- National Science Foundation
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g2(0) ∼ 0.2, and a decay constant of 2.75 ns that is further confirmed through fluorescence lifetime measurements. The results presented herein prove the existence of optically addressable isolated quantum emitters originating from defects in cBN, making this material an interesting platform for opto-electronic devices and quantum applications.
null (Ed.)van der Waals ferromagnets have gained significant interest due to their unique ability to provide magnetic response even at the level of a few monolayers. Particularly in combination with 2D semiconductors, such as the transition metal dichalcogenide WSe 2 , one can create heterostructures that feature unique magneto-optical response in the exciton emission through the magnetic proximity effect. Here we use 0D quantum emitters in WSe 2 to probe for the ferromagnetic response in heterostructures with Fe 3 GT and Fe 5 GT ferromagnets through an all-optical read-out technique that does not require electrodes. The spectrally narrow spin-doublet of the WSe 2 quantum emitters allowed to fully resolve the hysteretic magneto-response in the exciton emission, revealing the characteristic signature of both ferro- and antiferromagnetic proximity coupling that originates from the interplay among Fe 3 GT or Fe 5 GT, a thin surface oxide, and the spin doublets of the quantum emitters. Our work highlights the utility of 0D quantum emitters for probing interface magnetic dipoles in vdW heterostructures with high precision. The observed hysteretic magneto response in the exciton emission of quantum emitters adds further new degrees of freedom for spin and g -factor manipulation of quantum states.more » « less
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