Large optical nonlinearity of nanoantennas coupled to an epsilon-near-zero material

The size and operating energy of a nonlinear optical device are fundamentally constrained by the weakness of the nonlinear optical response of common materials1. Here, we report that a 50-nm-thick optical metasurface made of optical dipole antennas coupled to an epsilon-near-zero material exhibits a broadband (∼400 nm bandwidth) and ultrafast (recovery time less than 1 ps) intensity-dependent refractive index n2 as large as −3.73 ± 0.56 cm2 GW−1. Furthermore, the metasurface exhibits a maximum optically induced refractive index change of ±2.5 over a spectral range of ∼200 nm. The inclusion of low-Q nanoantennas on an epsilon-near-zero thin film not only allows the design of a metasurface with an unprecedentedly large nonlinear optical response, but also offers the flexibility to tailor the sign of the response. Our technique removes a longstanding obstacle in nonlinear optics: the lack of materials with an ultrafast nonlinear contribution to refractive index on the order of unity. It consequently offers the possibility to design low-power nonlinear nano-optical devices with orders-of-magnitude smaller footprints.PostprintPeer reviewe

Fabrication and characterization of plasmonic nanocone antennas for strong spontaneous emission enhancement

Plasmonic antennas are attractive nanostructures for a large variety of studies ranging from fundamental aspects of light matter interactions at the nanoscale to industry relevant applications such as ultrasensitive sensing, enhanced absorption in solar cells or solar fuel generation. A particularly interesting feature of these antennas is that they can enhance the fluorescence properties of emitters. Theoretical calculations have shown that nanocone antennas provide ideal results, but a high degree of manufacturing precision and control is needed to reach optimal performance. In this study, we report on the fabrication of nanocones with base diameters and heights in the range of 100 nm with variable aspect ratios using focused ion beam milling of sputtered nano crystalline gold layers. The controlled fabrication process allows us to obtain cones with tailored plasmon resonances. The measured plasmon spectra show very good agreement with finite difference time domain calculations. Theoretical investigations predict that these nanocones can enhance the spontaneous emission rate of a quantum emitter by several hundred times while keeping its quantum efficiency above 6

Strong Coupling between Self-Assembled Molecules and Surface Plasmon Polaritons

International audienceWe experimentally demonstrate strong coupling between self-assembled PTCDI-C7 organic molecules and the electromagnetic mode generated by surface plasmon polaritons (SPPs). The system consists of a dense self-assembly of ordered molecules evaporated directly on a thin gold film, which stack perpendicularly to the metal surface to form H-aggregates, without a host matrix. Experimental wavevector-resolved reflectance spectra show the formation of hybrid states that display a clear anticrossing, attesting the strong coupling regime with a Rabi splitting energy of ΩR ≃ 102 meV at room temperature. We demonstrate that the strength of the observed strong coupling regime derives from the high degree of organization of the dense layers of self-assembled molecules at the nanoscale that results in the concentration of the oscillator strength in a charge-transfer Frenkel exciton, with a dipole moment parallel to the direction of the maximum electric field. We compare our results to numerical simulations of a transfer matrix model and reach good qualitative agreement with the experimental findings. In our nanophotonic system, the use of self-assembled molecules opens interesting prospects in the context of strong coupling regimes with molecular systems

Epsilon-Near-Zero Strong Coupling in Metamaterial-Semiconductor Hybrid Structures

We present a new type of electrically tunable strong coupling between planar metamaterials and epsilon-near-zero modes that exist in a doped semiconductor nanolayer. The use of doped semiconductors makes this strong coupling tunable over a wide range of wavelengths through the use of different doping densities. We also modulate this coupling by depleting the doped semiconductor layer electrically. Our hybrid approach incorporates strong optical interactions into a highly tunable, integrated device platformclose191