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.
Chiral single photons are highly sought to enhance encoding capacities or enable propagation-dependent routing in nonreciprocal devices. Unfortunately, most semiconductor quantum emitters (QEs) produce only linear polarized photons unless external magnets are applied. Magnetic proximity coupling utilizing 2D ferromagnets promises to make bulky external fields obsolete. Here we directly grow Fe-doped MoS2(Fe:MoS2) via chemical vapor deposition that displays pronounced hard ferromagnetic properties even in monolayer form. This approach with monolayer ferromagnets enables full utilization of the strain from the pillar stressor to form QE in WSe2deterministically. The Fe:MoS2/WSe2heterostructures display strong hysteretic magneto-response and high-purity chiral single photons with a circular polarization degree of 92 ± 1% (74% average) without external magnetic fields. Furthermore, the chiral single photons are robust against uncontrolled twist-angle and external stray-fields. This ability to manipulate quantum states and transform linear polarized photons into high-purity chiral photons on-chip enables nonreciprocal device integration in quantum photonics.
more » « less- NSF-PAR ID:
- 10443871
- Publisher / Repository:
- IOP Publishing
- Date Published:
- Journal Name:
- 2D Materials
- Volume:
- 10
- Issue:
- 4
- ISSN:
- 2053-1583
- Page Range / eLocation ID:
- Article No. 045003
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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