Large Rabi splitting of mixed plasmon-exciton states in small plasmonic moiré cavities.

We report on exciton-plasmon coupling in metallic moiré cavities, both numerically and experimentally. Moiré cavities fabricated using double exposure laser interference lithography were filled with a molecular dye, J-aggregate. Polarization-dependent spectroscopic reflection measurements supported by simulations reveal strong coupling of organic dye excitons with cavity modes of the plasmonic moiré cavities. An anti-crossing at zero detuning, a clear indication of strong coupling, has been observed when the excitonic absorption band resonates with the cavity mode. Large Rabi splitting energies owing to the strong coupling of plasmons and excitons are clearly observed.

Focusing element formed by scattering structures in a planar dielectric waveguide.

A design process for creating integrated diffractive focusing elements for use in planar waveguides is presented. The elements consist of a linear array of holes etched into the core layer of a planar dielectric waveguide. A complete element is a few micrometers in size, while the individual holes are sub-micrometer. The focusing element was designed using analytical Mie theory. The performance of the complete 3D structure was then evaluated using 3D finite difference time domain (FDTD) method. A focal spot width of 227 nm (full width at half maximum) was predicted by 3D FDTD simulations with a peak intensity more than 10x the incident intensity and back-reflections lower than 1%. The focusing elements were fabricated using electron beam lithography and plasma etching. Fluorescence imaging was used to map the intensity in the waveguide core. The experimentally measured intensity maps were in good agreement with the simulations when the finite spatial resolution of the imaging system was taken into account.

Vertical Single-Crystalline Organic Nanowires on Graphene: Solution-Phase Epitaxy and Optical Microcavities.

Vertically aligned nanowires (NWs) of single crystal semiconductors have attracted a great deal of interest in the past few years. They have strong potential to be used in device structures with high density and with intriguing optoelectronic properties. However, fabricating such nanowire structures using organic semiconducting materials remains technically challenging. Here we report a simple procedure for the synthesis of crystalline 9,10-bis(phenylethynyl) anthracene (BPEA) NWs on a graphene surface utilizing a solution-phase van der Waals (vdW) epitaxial strategy. The wires are found to grow preferentially in a vertical direction on the surface of graphene. Structural characterization and first-principles ab initio simulations were performed to investigate the epitaxial growth and the molecular orientation of the BPEA molecules on graphene was studied, revealing the role of interactions at the graphene-BPEA interface in determining the molecular orientation. These free-standing NWs showed not only efficient optical waveguiding with low loss along the NW but also confinement of light between the two end facets of the NW forming a microcavity Fabry-Pérot resonator. From an analysis of the optical dispersion within such NW microcavities, we observed strong slowing of the waveguided light with a group velocity reduced to one-tenth the speed of light. Applications of the vertical single-crystalline organic NWs grown on graphene will benefit from a combination of the unique electronic properties and flexibility of graphene and the tunable optical and electronic properties of organic NWs. Therefore, these vertical organic NW arrays on graphene offer the potential for realizing future on-chip light sources.

Strong coupling between localized and propagating plasmon polaritons.

We investigate plasmon-plasmon (PP) coupling in the strongly interacting regimes by using a tunable plasmonic platform consisting of triangular Ag nanoprisms placed nanometers away from Ag thin films. The nanoprisms are colloidally synthesized using a seed-mediated growth method and having size-tunable localized surface plasmon polariton (SPP) resonances immobilized on Si(3)N(4) films. The PP coupling between the localized SPPs of metal nanoprisms and the propagating SPPs of the metal film is controlled by the nanoprism concentration and the plasmon damping in the metal film. Results reveal that Rabi splitting energy determining the strength of the coupling can reach up to several hundreds meV, thus demonstrating the ultrastrong coupling occurring between localized and propagating SPPs. The metal nanoparticle-metal thin film hybrid system over the square-centimeter areas presented here provides a unique configuration to study PP coupling all the way from the weak to ultrastrong coupling regimes in a broad range of wavelengths.

Plexcitonic crystals: a tunable platform for light-matter interactions.

Coupled states of surface plasmon polaritons (SPPs) and excitons are collectively called plexcitons [Nano Lett.8, 3481 (2008)]. Plexcitonics is an emerging field of research aiming to control light-matter interaction at the nanometer length scale using coupled pairs of surface-plasmons and excitons. Ability to control the interaction between localized excitons and propagating surface-plasmons is important for realization of new photonic devices. In this letter, we report plexcitonic crystals that yield direction-dependent plasmon-exciton coupling. We have fabricated one- and two-dimensional plexcitonic crystals on periodically corrugated silver surfaces, which are loaded with J-aggregate complexes. We show that plasmon-exciton coupling is blocked for some crystal directions when exciton energy falls inside the plasmonic band gap of the periodically corrugated metallic surface.

Plasmonic band gap engineering of plasmon-exciton coupling.

Controlling plasmon-exciton coupling through band gap engineering of plasmonic crystals is demonstrated in the Kretschmann configuration. When the flat metal surface is textured with a sinusoidal grating only in one direction, using laser interference lithography, it exhibits a plasmonic band gap because of the Bragg scattering of surface plasmon polaritons on the plasmonic crystals. The contrast of the grating profile determines the observed width of the plasmonic band gap and hence allows engineering of the plasmonic band gap. In this work, resonant coupling between the molecular resonance of a J-aggregate dye and the plasmonic resonance of a textured metal film is extensively studied through plasmonic band gap engineering. Polarization dependent spectroscopic reflection measurements probe the spectral overlap occurring between the molecular resonance and the plasmonic resonance. The results indicate that plasmon-exciton interaction is attenuated in the band gap region along the grating direction.

Absorption enhancement of molecules in the weak plasmon-exciton coupling regime.

We report on the experimental and theoretical investigations of enhancing the optical absorption of organic molecules in the weak plasmon-exciton coupling regime. A metal-organic hybrid structure consisting of dye molecules embedded in the polymer matrix is placed in close vicinity to thin metal films. We have observed a transition from a weak coupling regime to a strong coupling one as the thickness of the metal layer increases. The results indicate that absorption of the self-assembled J-aggregate nanostructures can be increased in the weak plasmon-exciton coupling regime and strongly quenched in the strong coupling regime. A theoretical model based on the transfer-matrix method qualitatively confirms the experimental results obtained from polarization-dependent spectroscopic reflection measurements.

Direct imaging of localized surface plasmon polaritons.

In this Letter, we report on dark field imaging of localized surface plasmon polaritons (SPPs) in plasmonic waveguiding bands formed by plasmonic coupled cavities. We image the light scattered from SPPs in the plasmonic cavities excited by a tunable light source. Tuning the excitation wavelength, we measure the localization and dispersion of the plasmonic cavity mode. Dark field imaging has been achieved in the Kretschmann configuration using a supercontinuum white-light laser equipped with an acoustooptic tunable filter. Polarization dependent spectroscopic reflection and dark field imaging measurements are correlated and found to be in agreement with finite-difference time-domain calculations.

Electrically switchable metadevices via graphene.

Metamaterials bring subwavelength resonating structures together to overcome the limitations of conventional materials. The realization of active metadevices has been an outstanding challenge that requires electrically reconfigurable components operating over a broad spectrum with a wide dynamic range. However, the existing capability of metamaterials is not sufficient to realize this goal. By integrating passive metamaterials with active graphene devices, we demonstrate a new class of electrically controlled active metadevices working in microwave frequencies. The fabricated active metadevices enable efficient control of both amplitude (>50 dB) and phase (>90°) of electromagnetic waves. In this hybrid system, graphene operates as a tunable Drude metal that controls the radiation of the passive metamaterials. Furthermore, by integrating individually addressable arrays of metadevices, we demonstrate a new class of spatially varying digital metasurfaces where the local dielectric constant can be reconfigured with applied bias voltages. In addition, we reconfigure resonance frequency of split-ring resonators without changing its amplitude by damping one of the two coupled metasurfaces via graphene. Our approach is general enough to implement various metamaterial systems that could yield new applications ranging from electrically switchable cloaking devices to adaptive camouflage systems.