We demonstrate the real-time exciton-manipulation of plexcitonic coupling in monolayer WS2 coupled to a plasmonic nanocavity by immersing into a mixed solution of dichloromethane (DCM) and ethanol. By adjusting the mixture ratio, a continuous tuning of the Rabi splitting energy ranged from 178 meV (in ethanol) to 266 meV (in DCM) is achieved. The results are mainly attributed to the remarkable increase of the proportion of neutral exciton in the monolayer WS2 (from 59% to 100%) as the concentration of DCM is increased. It offers an important stepping stone towards a further study of plexcitonic coupling in layered materials, along with potential applications in quantum information processing and nonlinear optical materials.
Transition-metal dichalcogenides with their exciton-dominated optical behavior emerge as promising materials for realizing strong light-matter interactions in the visible range and at ambient conditions. When these materials are combined with metals, the energy confining ability of plasmon polaritons in metals below the diffraction limit, allows for further enhancing and tailoring the light-matter interaction, due to the formation of plexcitons in hybrid metal-TMDC structures at the interface. Herein, we demonstrate that the coupling between quasi-propagating plasmons in plasmonic crystals and…
Compact electro-optic (EO) modulators with large extinction ratios, low-switching energies, and high operation speeds are desirable for integrated photonic and linear optical computing. Traditional 3D semiconductors and dielectrics are unsuitable for achieving such modulators due to the small magnitude of EO effects in them. Excitonic 2D semiconductors present a unique opportunity in this regard given their large and tunable optical constants near the excitonic resonances. However, strategies for confining and electrically tuning the excitons into compact EO modulators have not been realized t…
Plexcitonic strong coupling has ushered in an era of room-temperature quantum electrodynamics that is achievable at the nanoscale, with potential applications ranging from high-precision single-molecule spectroscopy to quantum technologies functional under ambient conditions. Realizing these applications on an industrial scale requires scalable and mass-producible plasmonic cavities that provide ease of access and control for quantum emitters. Via a rational selection of substrates and the canonical gold bowtie nanoantenna, we propose a novel design strategy for multidimensional engineering of…
Establishing a coherent interaction between a material resonance and an optical cavity is a necessary first step for the development of semiconductor quantum optics. Here we demonstrate a coherent interaction between the neutral exciton in monolayer MoSe2 and a zero-dimensional, small mode volume nanocavity. This is observed through a dispersive shift of the cavity resonance when the exciton-cavity detuning is decreased, with an estimated exciton-cavity coupling of ~4.3 meV and a cooperativity of C~3.4 at 80 Kelvin. This coupled exciton-cavity platform is expected to reach the strong light-mat…
Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features i…
Hybrid photonic structures of plasmonic metasurfaces coupled to atomically thin semiconductors have emerged as a versatile platform for strong light-matter interaction, supporting both strong coupling and parametric nonlinearities. However, designing optimized nonlinear hybrid metasurfaces is a complex task, as the multiple parameters' contribution to the nonlinear response is elusive. Here we present a simple yet powerful strategy for maximizing the nonlinear response of the hybrid structures based on evolutionary inverse design of the metasurface's near-field enhancement around the excitonic…
Plasmonic cavities can be used to control the atom-photon coupling process at the nanoscale, since they provide ultrahigh density of optical states in an exceptionally small mode volume. Here we demonstrate strong coupling between molecular excitons and plasmonic resonances (so-called plexcitonic coupling) in a film-coupled nanocube cavity, which can induce profound and significant spectral and spatial modifications to the plasmonic gap modes. Within the spectral span of a single gap mode in the nanotube-film cavity with a 3-nm wide gap, the introduction of narrow-band J-aggregate dye molecule…
Two-photon Rabi splitting in a cavity-dot system provides a basis for multi-qubit coherent control in quantum photonic network. Here we report on two-photon Rabi splitting in a strongly coupled cavity-dot system. The quantum dot was grown intentionally large in size for large oscillation strength and small biexciton binding energy. Both exciton and biexciton transitions couple to a high quality factor photonic crystal cavity with large coupling strengths over 130 $μ$eV. Furthermore, the small binding energy enables the cavity to simultaneously couple with two exciton states. Thereby two-photon…
The phase delay of a local electric field, being well-known in plasmonic nanostructures, has seldom been investigated to modulate the plasmon-exciton interaction. Here, with the single-particle spectroscopy method, we experimentally investigate the phase effect in plasmon-exciton coupling systems consisting of monolayer WSe2 and an individual gold nanorod. The local plasmon phase delay is tuned by adopting various nanorods with different resonant energies respective to the exciton. We find that the local plasmon phase delay between the excitons and the plasmonic modes is as equally essential a…
In this paper, we report theoretical investigation on excitation of surface plexciton wave at interface of a metal and a columnar thin film infiltrated with J-aggregate dyes using transfer matrix method in Kretschmann configuration. The results reveal the regime of the plasmon - exciton interaction can change from weak to strong by tuning structural parameters. We find Rabi splitting energies between 204 -378 meV corresponding to the time period 11-20 fs which includes to the fast energy transfer from surface plasmon polaritons to excitons. The phase speed and propagation length of surface ple…
We theoretically analyse the hybrid Mie-exciton optical modes arising from the strong coupling of excitons in organic dyes or transition-metal dichalcogenides with the Mie resonances of high-index dielectric nanoparticles. Detailed analytic calculations show that silicon--exciton core--shell nanoparticles are characterised by a richness of optical modes which can be tuned through nanoparticle dimensions to produce large anticrossings in the visible or near infrared, comparable to those obtained in plexcitonics. The complex magnetic-excitonic nature of these modes is understood through spectral…
Strong exciton-plasmon interaction between the layered two-dimensional (2D) semiconductors and gap plasmons shows a great potential to implement cavity quantum-electrodynamics in ambient condition. However, achieving a robust plasmon-exciton coupling with nanocavity is still very challenging, because the layer area is usually small with conventional approaches. Here, we report on a robust strong exciton-plasmon coupling between the gap mode of bowtie and the excitons in MoS$_2$ layers with gold-assisted mechanical exfoliation and the nondestructive wet transfer techniques for large-area layer.…
