Monolayer transition metal dichalcogenides (TMDCs) have recently been proposed as a unique excitonic platform for advanced optical and electronic functionalities. However, in spite of intense research efforts, it has been largely overlooked that, in addition to displaying rich exciton physics, TMDCs also possess a very high refractive index. This opens a possibility to utilize these materials for constructing resonant nanoantennas based on subwavelength geometrical modes. Here we show that nanodisks fabricated from exfoliated multilayer WS 2 support distinct Mie resonances and so-called anapole states that can be easily tuned in wavelength over the visible and near-infrared spectral range by varying the nanodisks' size and aspect ratio. We argue that the TMDC material anisotropy and the presence of excitons substantially enrich nanophotonics by complementing traditional approaches based on plasmonics and well-known high-index materials such as silicon. As a proof-of-concept, we demonstrate a novel regime of light-matter interaction, anapole-exciton polaritons, which we realize within a single WS 2 nanodisk. Our results thus suggest that nanopatterned TMDCs are promising materials for high-index nanophotonics applications with enriched functionalities and superior prospects.
Strong coupling of organic chromophores to plasmonic nanoparticles was shown to markedly improve molecular photostability.
Monolayer transition-metal dichalcogenides (TMDCs) have attracted a lot of research attention recently, motivated by their remarkable optical properties and potential for strong light-matter interactions. Realization of strong plasmon-exciton coupling is especially desirable in this context because it holds promise for the enabling of room-temperature quantum and nonlinear optical applications. These efforts naturally require investigations at a single-nanoantenna level, which, in turn, should possess a compact optical mode interacting with a small amount of excitonic material. However, standard plasmonic nanoantenna designs such as nanoparticle dimers or particle-on-film suffer from misalignment of the local electric field in the gap with the in-plane transition dipole moment of monolayer TMDCs. Here, we circumvent this problem by utilizing gold bi-pyramids (BPs) as very efficient plasmonic nanoantennas. We demonstrate strong coupling between individual BPs and tungsten diselenide (WSe) monolayers at room temperature. We further study the coupling between multilayers of WSe and BPs to elucidate the effect of the number of layers on the coupling strength. Importantly, BPs adopt a reduced-symmetry configuration when deposited on WSe, such that only one sharp antenna tip efficiently interacts with excitons. Despite the small interaction area, we manage to achieve strong coupling, with Rabi splitting exceeding ∼100 meV. Our results suggest a feasible way toward realizing plasmon-exciton polaritons involving nanoscopic areas of TMDCs, thus pointing toward quantum and nonlinear optics applications at ambient conditions.
Halide perovskites are known to support excitons at room temperatures with high quantum yield of luminescence that make them attractive for all-dielectric resonant nanophotonics and meta-optics. Here we report the observation of broadly tunable Fano resonances in halide perovskite nanoparticles originating from the coupling of excitons to the Mie resonances excited in the nanoparticles. Signatures of the photon-exciton (" hybrid") Fano resonances are observed in dark-field spectra of isolated nanoparticles, and also in the extinction spectra of aperiodic lattices of such nanoparticles. In the latter case, chemical tunability of the exciton resonance allows reversible tuning of the Fano resonance across the 100 nm bandwidth in the visible frequency range, providing a novel approach to control optical properties of perovskite nanostructures. The proposed method of chemical tuning paves the way to an efficient control of emission properties of on-chip-integrated light-emitting nanoantennas.
Transition metal dichalcogenides (TMDCs) have attracted significant attention recently in the context of strong light–matter interaction. To observe strong coupling using these materials, excitons are typically hybridized with resonant photonic modes of stand-alone optical cavities, such as Fabry–Pérot microcavities or plasmonic nanoantennas. Here, we show that thick flakes of layered van der Waals TMDCs can themselves serve as low-quality resonators due to their high background permittivity. Optical modes of such “cavities” can in turn hybridize with excitons in the same material. We perform an experimental and theoretical study of such self-hybridization in thick flakes of four common TMDC materials: WS2, WSe2, MoS2, and MoSe2. We observe splitting in reflection and transmission spectra in all four cases and provide angle-resolved dispersion measurements of exciton-polaritons as well as thickness-dependent data. Moreover, we observe significant enhancement and broadening of absorption in thick TMDC multilayers, which can be interpreted in terms of strong light–matter coupling. Remarkably, absorption reaches >50% efficiency across the entire visible spectrum, while simultaneously being weakly dependent on polarization and angle of incidence. Our results thus suggest formation of self-hybridized exciton-polaritons in thick TMDC flakes, which in turn may pave the way toward polaritonic and optoelectronic devices in these simple systems.
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