Optically active defects in 2D materials, such as hexagonal boron nitride (hBN) and transition metal dichalcogenides (TMDs), are an attractive class of single-photon emitters with high brightness, room-temperature operation, site-specific engineering of emitter arrays, and tunability with external strain and electric fields. In this work, we demonstrate a novel approach to precisely align and embed hBN and TMDs within background-free silicon nitride microring resonators. Through the Purcell effect, high-purity hBN emitters exhibit a cavity-enhanced spectral coupling efficiency up to 46% at room temperature, which exceeds the theoretical limit for cavity-free waveguide-emitter coupling and previous demonstrations by nearly an order-of-magnitude. The devices are fabricated with a CMOS-compatible process and exhibit no degradation of the 2D material optical properties, robustness to thermal annealing, and 100 nm positioning accuracy of quantum emitters within single-mode waveguides, opening a path for scalable quantum photonic chips with on-demand single-photon sources.
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Defect and strain engineering of monolayer WSe2 enables site-controlled single-photon emission up to 150 K
Abstract In recent years, quantum-dot-like single-photon emitters in atomically thin van der Waals materials have become a promising platform for future on-chip scalable quantum light sources with unique advantages over existing technologies, notably the potential for site-specific engineering. However, the required cryogenic temperatures for the functionality of these sources has been an inhibitor of their full potential. Existing methods to create emitters in 2D materials face fundamental challenges in extending the working temperature while maintaining the emitter’s fabrication yield and purity. In this work, we demonstrate a method of creating site-controlled single-photon emitters in atomically thin WSe 2 with high yield utilizing independent and simultaneous strain engineering via nanoscale stressors and defect engineering via electron-beam irradiation. Many of the emitters exhibit biexciton cascaded emission, single-photon purities above 95%, and working temperatures up to 150 K. This methodology, coupled with possible plasmonic or optical micro-cavity integration, furthers the realization of scalable, room-temperature, and high-quality 2D single- and entangled-photon sources.
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- Award ID(s):
- 2032272
- NSF-PAR ID:
- 10249242
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract 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.
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Abstract 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.
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Abstract High-precision placement of rare-earth ions in scalable silicon-based nanostructured materials exhibiting high photoluminescence (PL) emission, photostable and polarized emission, and near-radiative-limited excited state lifetimes can serve as critical building blocks toward the practical implementation of devices in the emerging fields of nanophotonics and quantum photonics. Introduced herein are optical nanostructures composed of arrays of ultrathin silicon carbide (SiC) nanowires (NWs) that constitute scalable one-dimensional NW-based photonic crystal (NW-PC) structures. The latter are based on a novel, fab-friendly, nanofabrication process. The NW arrays are grown in a self-aligned manner through chemical vapor deposition. They exhibit a reduction in defect density as determined by low-temperature time-resolved PL measurements. Additionally, the NW-PC structures enable the positioning of erbium (Er 3+ ) ions with an accuracy of 10 nm, an improvement on the current state-of-the-art ion implantation processes, and allow strong coupling of Er 3+ ions in NW-PC. The NW-PC structure is pivotal in engineering the Er 3+ -induced 1540-nm emission, which is the telecommunication wavelength used in optical fibers. An approximately 60-fold increase in the room-temperature Er 3+ PL emission is observed in NW-PC compared to its thin-film analog in the linear pumping regime. Furthermore, 22 times increase in the Er 3+ PL intensity per number of exited Er ions in NW-PC was observed at saturation while using 20 times lower pumping power. The NW-PC structures demonstrate broadband and efficient excitation characteristics for Er 3+ , with an absorption cross-section (~2 × 10 −18 cm 2 ) two-order larger than typical benchmark values for direct absorption in rare-earth-doped quantum materials. Experimental and simulation results show that the Er 3+ PL is photostable at high pumping power and polarized in NW-PC and is modulated with NW-PC lattice periodicity. The observed characteristics from these technologically friendly nanophotonic structures provide a promising route to the development of scalable nanophotonics and formation of single-photon emitters in the telecom optical wavelength band.more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41467-021-23709-5
