Optical nanoantennas provide control of light at the nanoscale, which makes them important for diverse areas ranging from photocatalysis and flat metaoptics to sensors and biomolecular tweezing. They have traditionally been limited to metallic and dielectric nanostructures that sustain plasmonic and Mie resonances, respectively. More recently, nanostructures of organic J-aggregate excitonic materials have been proposed capable of also supporting nanooptical resonances, although their advance has been hampered from difficulty in nanostructuring. Here, the authors present the realization of organic J-aggregate excitonic nanostructures, using nanocylinder arrays as model system. Extinction spectra show that they can sustain both plasmon-like resonances and dielectric resonances, owing to the material providing negative and large positive permittivity regions at the different sides of its exciton resonance. Furthermore, it is found that the material is highly anisotropic, leading to hyperbolic and elliptic permittivity regions. Nearfield analysis using optical simulation reveals that the nanostructures therefore support hyperbolic localized surface exciton resonances and elliptic Mie resonances, neither of which has been previously demonstrated for this type of material. The anisotropic nanostructures form a new type of optical nanoantennas, which combined with the presented fabrication process opens up for applications such as fully organic excitonic metasurfaces.

Being able to dynamically shape light at the nanoscale is oneof the ultimate goals in nano-optics1. Resonant light–matterinteraction can be achieved using conventional plasmonicsbased on metal nanostructures, but their tunability is highlylimited due to a fixed permittivity2. Materials with switchablestates and methods for dynamic control of light–matterinteraction at the nanoscale are therefore desired. Here weshow that nanodisks of a conductive polymer can supportlocalized surface plasmon resonances in the near-infraredand function as dynamic nano-optical antennas, with their resonancebehaviour tunable by chemical redox reactions. Theseplasmons originate from the mobile polaronic charge carriersof a poly(3,4-ethylenedioxythiophene:sulfate) (PEDOT:Sulf)polymer network. We demonstrate complete and reversibleswitching of the optical response of the nanoantennasby chemical tuning of their redox state, which modulatesthe material permittivity between plasmonic and dielectricregimes via non-volatile changes in the mobile chargecarrier density. Further research may study different conductivepolymers and nanostructures and explore their usein various applications, such as dynamic meta-optics andreflective displays.

The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) forms a promising alternative to conventional inorganic conductors, where deposition of thin films via vapour phase polymerization (VPP) has gained particular interest owing to high electrical conductivity within the plane of the film. The conductivity perpendicular to the film is typically much lower, which may be related not only to preferential alignment of PEDOT crystallites but also to vertical stratification across the film. In this study, we reveal non-linear vertical microstructural variations across VPP PEDOT:Tos thin films, as well as significant differences in doping level between the top and bottom surfaces. The results are consistent with a VPP mechanism based on diffusion-limited transport of polymerization precursors. Conducting polymer films with vertical inhomogeneity may find applications in gradient-index optics, functionally graded thermoelectrics, and optoelectronic devices requiring gradient doping.

Plasmonic metasurfaces based on ensembles of distributed metallic nanostructures can absorb, scatter, and in other ways shape light at the nanoscale. Forming hybrid plasmonic metasurfaces by combination with other materials opens up for new research directions and novel applications. This perspective highlights some of the recent advancements in this vibrant research field. Particular emphasis is put on hybrid plasmonic metasurfaces comprising organic materials and on concepts related to switchable surfaces, light-to-heat conversion, and hybridized light-matter states based on strong coupling.

Solid state nanopores are central structures for many applications. To date, much effort has been spent on controlled fabrication of single nanopores, while relatively little work has focused on large scale fabrication of arrays of nanopores. In this work we show wafer-scale fabrication of plasmonic nanopores in 50 nm thick silicon nitride membranes with one or two 30 nm gold films, using electron beam lithography with a negative resist or a new version of colloidal lithography. Both approaches offer good control of pore diameter (even below 100 nm) and with high yield (>90%) of intact membranes. Colloidal lithography has the advantage of parallel patterning without expensive equipment. Despite its serial nature, electron beam lithography provides high throughput and can make arbitrary array patterns. Importantly, both methods prevent metal from ending up on the membrane pore sidewalls. The new fabrication methods make it possible to compare the optical properties of structurally identical plasmonic nanopore arrays with either long-range order (e-beam) or short-range order (colloidal). The resonance features in the extinction spectrum are very similar for both structures when the pitch is the same as the characteristic spacing in the self-assembled colloidal pattern. Long-range ordering slightly enhances the magnitude of the extinction maximum and blueshift the transmission maximum by tens of nm. Upon reducing the diameter in long-range ordered arrays, the resonance is reduced in magnitude and the transmission maximum is further blue shifted, just like for short-range ordered arrays. These effects are well explained by interpreting the spectra as Fano interference between the grating-type excitation of propagating surface plasmons and the broad transmission via individual pores in the metal film. Furthermore, we find that only the short-range ordered arrays scatter light, which we attribute to the highly limited effective period in the short-range ordered system and the corresponding lack of coherent suppression of scattering via interference effects.

Plasmons and excitons can interact to form new hybridized light–matter states, with a multitude of potential applications including optical logic circuits and single-photon switches. Here, we report the first observation of strong coupling based on optically thin plasmonic nanohole films. The absorptive plasmon resonances of these nanohole films lead to suppressed transmission and Fano-shaped extinction peaks. We prepared silver nanohole films by colloidal lithography, which enables large-scale fabrication of nanoholes distributed in a short-range order. When coated with J-aggregate molecules, both extinction and absorption spectra show clear formation of two separated polariton resonances, with vacuum Rabi splitting on the order of 300 meV determined from anticrossing experiments. In accordance with strong coupling theory, the splitting magnitude increases linearly with the square root of molecular concentration. The extinction peak positions are blue-shifted from the absorption polariton positions, as explained by additional Fano interference between the hybridized states and the metal film. This highlights that absorption measurements are important not only to prove strong coupling but also to correctly determine hybridized polariton positions and splitting magnitudes in hybrid plasmonic nanohole systems. The polariton absorption peaks also show strong dependence on illumination direction, as found related to inherent directionality of the plasmonic nanohole metasurface and differences in light interaction with nonhybridized molecules. Importantly, optical simulations could successfully reproduce the experimental results and all coupling features. Furthermore, simulated spatial distribution of the absorption provides additional evidence of strong coupling in the hybrid nanohole system. The work paves the way toward strong coupling applications based on optically thin nanohole systems, as further promoted by the scalable fabrication.