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
Magnesium vanadate (MgV2O6) and its alloys with copper vanadate were synthesized via the solution combustion technique. Phase purity and solid solution formation were confirmed by a variety of experimental techniques, supported by electronic structure simulations based on density functional theory (DFT). Powder X-ray diffraction combined with Rietveld refinement, laser Raman spectroscopy, diffuse reflectance spectroscopy, and high-resolution transmission electron microscopy showed single-phase alloy formation despite the MgV2O6 and CuV2O6 end members exhibiting monoclinic and triclinic crystal systems, respectively. DFT-calculated optical band gaps showed close agreement in the computed optical bandgaps with experimentally derived values. Surface photovoltage spectroscopy, ambient-pressure photoemission spectroscopy, and Kelvin probe contact potential difference (work function) measurements confirmed a systematic variation in the optical bandgap modification and band alignment as a function of stoichiometry in the alloy composition. These data indicated n-type semiconductor behavior for all the samples which was confirmed by photoelectrochemical measurements.
RESUMEN
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 WSe2 through 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 WSe2 is simplified into spectrally isolated SPEs with high single-photon purity. Density functional theory calculations reveal energetic alignment between WSe2 defect 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.
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
Surface-enhanced Raman spectroscopy (SERS) is a widely used sensing technique for ultrasensitivity chemical sensing, biomedical detection, and environmental analysis. Because SERS signal is proportional to the fourth power of the local electric field, several SERS applications have focused on the design of plasmonic nanogaps to take advantage of the extremely strong near-field enhancement that results from plasmonic coupling, but few designs have focused on how SERS detection is affected by molecular orientation within these nanogaps. Here, we demonstrate a nanoparticle-on-metal metasurface designed for near-perfect optical absorption as a platform for Raman detection of highly oriented molecular analytes, including two-dimensional materials and aromatic molecules. This metasurface platform overcomes challenges in nanoparticle aggregation, which commonly leads to low or fluctuating Raman signals in other colloidal nanoparticle platforms. Our metasurface-enhanced Raman spectroscopy (mSERS) platform is based on a colloidal Langmuir-Schaefer deposition, with up to 32% surface coverage density of nanogaps across an entire sensor chip. In this work, we perform both simulations of the local electric field and experimental characterization of the mSERS signal obtained for oriented molecular layers. We then demonstrate this mSERS platform for the quantitative detection of the drinking-water toxin polybrominated diphenyl ether (BDE-15), with a limit of detection of 0.25 µM under 530 µW excitation. This detection limit is comparable to other SERS-based sensors operating at laser powers over 3 orders of magnitude higher, indicating the promise of our mSERS platform for nondestructive and low-level analyte detection.
