RESUMEN
Strain-engineering in atomically thin metal dichalcogenides is a useful method for realizing single-photon emitters (SPEs) for quantum technologies. Correlating SPE position with local strain topography is challenging due to localization inaccuracies from the diffraction limit. Currently, SPEs are assumed to be positioned at the highest strained location and are typically identified by randomly screening narrow-linewidth emitters, of which only a few are spectrally pure. In this work, hyperspectral quantum emitter localization microscopy is used to locate 33 SPEs in nanoparticle-strained WSe2 monolayers with sub-diffraction-limit resolution (≈30 nm) and correlate their positions with the underlying strain field via image registration. In this system, spectrally pure emitters are not concentrated at the highest strain location due to spectral contamination; instead, isolable SPEs are distributed away from points of peak strain with an average displacement of 240 nm. These observations point toward a need for a change in the design rules for strain-engineered SPEs and constitute a key step toward realizing next-generation quantum optical architectures.
RESUMEN
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, WSe2 monolayers (MLs) are promising for the deterministic fabrication and engineering of SPEs using local strain fields. The ability to reliably produce isolatable SPEs in WSe2 is 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 WSe2 MLs, 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 WSe2 MLs 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.
RESUMEN
Colloidal semiconductor nanoplatelets (NPLs) are a scalable materials platform for optoelectronic applications requiring fast and narrow emission, including spin-to-photon transduction within quantum information networks. In particular, three-particle negative trions of NPLs are appealing emitters since, unlike excitons, they do not have an optically "dark" sublevel. In CdSe NPLs, trion emission dominates the photoluminescence (PL) spectrum at low temperature but using them as single photon-emitting states requires more knowledge about their preparation, since trions in these materials are not directly optically accessible from the ground state. This work demonstrates, using power-dependent time-resolved transient absorptions (TA) of CdSe NPLs, that trions form via biexciton decay in 1.6 ps. The scaling of the trion population and formation lifetime with excitation power indicates that they do not form through collisional mechanisms typical for 2D materials, but rather by a unimolecular hole transfer. This work is a step toward deterministic single photon emission from trions.
