Lead halide perovskite nanocrystals (NCs) are emerging as optically active materials for solution-processed optoelectronic devices. Despite the technological relevance of tracing rational guidelines for optimizing their performances and stability beyond their intrinsic resilience to structural imperfections, no in-depth study of the role of selective carrier trapping and environmental conditions on their exciton dynamics has been reported to date. Here we conduct spectro-electrochemical (SEC) experiments, side-by-side to oxygen sensing measurements on CsPbBr NCs for the first time. We show that the application of EC potentials controls the emission intensity by altering the occupancy of defect states without degrading the NCs. Reductive potentials lead to strong (60%) emission quenching by trapping of photogenerated holes, whereas the concomitant suppression of electron trapping is nearly inconsequential to the emission efficiency. Consistently, oxidizing conditions result in minor (5%) brightening due to suppressed hole trapping, confirming that electron traps play a minor role in nonradiative decay. This behavior is rationalized through a model that links the occupancy of trap sites with the position of the NC Fermi level controlled by the EC potential. Photoluminescence measurements in controlled atmosphere reveal strong quenching by collisional interactions with O, which is in contrast to the photobrightening effect observed in films and single crystals. This indicates that O acts as a scavenger of photoexcited electrons without mediation by structural defects and, together with the asymmetrical SEC response, suggests that electron-rich defects are likely less abundant in nanostructured perovskites than in the bulk, leading to an emission response dominated by direct interaction with the environment.

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.

Nanostructured surfaces with designed optical functionalities, such as metasurfaces, allow efficient harvesting of light at the nanoscale, enhancing light–matter interactions for a wide variety of material combinations. Exploiting light-driven matter excitations in these artificial materials opens up a new dimension in the conversion and management of energy at the nanoscale. In this review, we outline the impact, opportunities, applications, and challenges of optical metasurfaces in converting the energy of incoming photons into frequency-shifted photons, phonons, and energetic charge carriers. A myriad of opportunities await for the utilization of the converted energy. Here we cover the most pertinent aspects from a fundamental nanoscopic viewpoint all the way to applications.

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.

All-dielectric nanophotonics underpinned by the physics of bound states in the continuum (BICs) have demonstrated breakthrough applications in nanoscale light manipulation, frequency conversion and optical sensing. Leading BIC implementations range from isolated nanoantennas with localized electromagnetic fields to symmetry-protected metasurfaces with controllable resonance quality (Q) factors. However, they either require structured light illumination with complex beam-shaping optics or large, fabrication-intense arrays of polarization-sensitive unit cells, hindering tailored nanophotonic applications and on-chip integration. Here, we introduce radial quasi-bound states in the continuum (radial BICs) as a new class of radially distributed electromagnetic modes controlled by structural asymmetry in a ring of dielectric rod pair resonators. The radial BIC platform provides polarization-invariant and tunable high-Q resonances with strongly enhanced near fields in an ultracompact footprint as low as 2 µm2. We demonstrate radial BIC realizations in the visible for sensitive biomolecular detection and enhanced second-harmonic generation from monolayers of transition metal dichalcogenides, opening new perspectives for compact, spectrally selective, and polarization-invariant metadevices for multi-functional light-matter coupling, multiplexed sensing, and high-density on-chip photonics.

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.

Self-assembly of excitonic nanostructures from excess cationic MAI:PbCl2 perovskite solutions.