Unique structural and optical properties of atomically thin two-dimensional semiconducting transition metal dichalcogenides enable in principle their efficient coupling to photonic cavities having the optical mode volume close to or below the diffraction limit. Recently, it has become possible to make all-dielectric nano-cavities with reduced mode volumes and negligible non-radiative losses. Here, we realise low-loss high-refractive-index dielectric gallium phosphide (GaP) nano-antennas with small mode volumes coupled to atomic mono- and bilayers of WSe. We observe a photoluminescence enhancement exceeding 10 compared with WSe placed on planar GaP, and trace its origin to a combination of enhancement of the spontaneous emission rate, favourable modification of the photoluminescence directionality and enhanced optical excitation efficiency. A further effect of the coupling is observed in the photoluminescence polarisation dependence and in the Raman scattering signal enhancement exceeding 10. Our findings reveal dielectric nano-antennas as a promising platform for engineering light-matter coupling in two-dimensional semiconductors.

Atomically thin two-dimensional semiconducting transition metal dichalcogenides (TMDs) can withstand large levels of strain before their irreversible damage occurs. This unique property offers a promising route for control of the optical and electronic properties of TMDs, for instance, by depositing them on nanostructured surfaces, where position-dependent strain can be produced on the nanoscale. Here, we demonstrate strain-induced modifications of the optical properties of mono-and bilayer TMD WSe 2 placed on photonic nanoantennas made from gallium phosphide (GaP). Photoluminescence (PL) from the strained areas of the TMD layer is enhanced owing to the efficient coupling with the confined optical mode of the nanoantenna. Thus, by following the shift of the PL peak, we deduce the changes in the strain in WSe 2 deposited on the nanoantennas of different radii. In agreement with the presented theory, strain up to ≈1.4% is observed for WSe 2 monolayers. We also estimate that >3% strain is achieved in bilayers, accompanied by the emergence of a direct bandgap in this normally indirect-bandgap semiconductor. At cryogenic temperatures, we find evidence of the exciton confinement in the most strained nanoscale parts of the WSe 2 layers, as also predicted by our theoretical model. Our results of direct relevance for both dielectric and plasmonic nanoantennas, show that strain in atomically thin semiconductors can be used as an additional parameter for engineering light−matter interaction in nanophotonic devices.

Single photon emitters in atomically-thin semiconductors can be deterministically positioned using strain induced by underlying nano-structures. Here, we couple monolayer WSe2 to high-refractive-index gallium phosphide dielectric nano-antennas providing both optical enhancement and monolayer deformation. For single photon emitters formed on such nano-antennas, we find very low (femto-Joule) saturation pulse energies and up to 104 times brighter photoluminescence than in WSe2 placed on low-refractive-index SiO2 pillars. We show that the key to these observations is the increase on average by a factor of 5 of the quantum efficiency of the emitters coupled to the nano-antennas. This further allows us to gain new insights into their photoluminescence dynamics, revealing the roles of the dark exciton reservoir and Auger processes. We also find that the coherence time of such emitters is limited by intrinsic dephasing processes. Our work establishes dielectric nano-antennas as a platform for high-efficiency quantum light generation in monolayer semiconductors.

Transition metal dichalcogenides have emerged as promising materials for nanophotonic resonators because of their large refractive index, low absorption within a large portion of the visible spectrum, and compatibility with a wide range of substrates. Herein, we use these properties to fabricate WS 2 double-pillar nanoantennas in a variety of geometries enabled by the anisotropy in the crystal structure. Using dark-field spectroscopy, we reveal multiple Mie resonances, to which we couple WSe 2 monolayer photoluminescence and achieve Purcell enhancement and an increased fluorescence by factors up to 240 for dimer gaps of 150 nm. We introduce postfabrication atomic force microscope repositioning and rotation of dimer nanoantennas, achieving gaps as small as 10 ± 5 nm, which enables a host of potential applications, including strong Purcell enhancement of single-photon emitters and optical trapping, which we study in simulations. Our findings highlight the advantages of using transition metal dichalcogenides for nanophotonics by exploring applications enabled by their properties.

Focused ion beam (FIB) is an effective tool for precise nanoscale fabrication. It has recently been employed to tailor defect engineering in functional nanomaterials such as two-dimensional transition metal dichalcogenides (TMDCs), providing desirable properties in TMDC-based optoelectronic devices. However, the damage caused by the FIB irradiation and milling process to these delicate, atomically thin materials, especially in extended areas beyond the FIB target, has not yet been fully characterised. Understanding the correlation between lateral ion beam effects and optical properties of 2D TMDCs is crucial in designing and fabricating high-performance optoelectronic devices. In this work, we investigate lateral damage in large-area monolayer WS2 caused by the gallium focused ion beam milling process. Three distinct zones away from the milling location are identified and characterised via steady-state photoluminescence (PL) and Raman spectroscopy. The emission in these three zones have different wavelengths and decay lifetimes. An unexpected bright ring-shaped emission around the milled location has also been revealed by time-resolved PL spectroscopy with high spatial resolution. Our findings open up new avenues for tailoring the optical properties of TMDCs by charge and defect engineering via focused ion beam lithography. Furthermore, our study provides evidence that while some localised damage is inevitable, distant destruction can be eliminated by reducing the ion beam current. It paves the way for the use of FIB to create nanostructures in 2D TMDCs, as well as the design and realisation of optoelectrical devices on a wafer scale.

Numerous optical phenomena and applications have been enabled by nanophotonic structures. Their current fabrication from high refractive index dielectrics, such as silicon (Si) or gallium phosphide (GaP), pose restricting fabrication challenges while metals, relying on plasmons and thus exhibiting high ohmic losses, limit the achievable applications. An emerging class of layered, so‐called van der Waals (vdW), crystals is presented as a viable nanophotonics platform in this work. The dielectric response of 11 mechanically exfoliated thin‐film (20–200 nm) vdW crystals is extracted, revealing high refractive indices up to n = 5, pronounced birefringence up to Δn = 3, sharp absorption resonances, and a range of transparency windows from ultraviolet to near‐infrared. Nanoantennas are subsequently fabricated on silicon dioxide (SiO2) and gold, utilizing the compatibility of vdW thin films with a variety of substrates. Pronounced Mie resonances are observed due to the high refractive index contrast on SiO2, leading to a strong exciton‐photon coupling regime as well as largely unexplored high‐quality‐factor, hybrid Mie‐plasmon modes on gold. Additional vdW‐material‐specific degrees of freedom in fabrication are further demonstrated by realizing nanoantennas from stacked twisted crystalline thin‐films, enabling control of nonlinear optical properties, and post‐fabrication nanostructure transfer, important for nano‐optics with sensitive materials.

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