Ultrastrong coupling between nanoparticle plasmons and cavity photons at ambient conditions.

Ultrastrong coupling is a distinct regime of electromagnetic interaction that enables a rich variety of intriguing physical phenomena. Traditionally, this regime has been reached by coupling intersubband transitions of multiple quantum wells, superconducting artificial atoms, or two-dimensional electron gases to microcavity resonators. However, employing these platforms requires demanding experimental conditions such as cryogenic temperatures, strong magnetic fields, and high vacuum. Here, we use a plasmonic nanorod array positioned at the antinode of a resonant optical Fabry-Pérot microcavity to reach the ultrastrong coupling (USC) regime at ambient conditions and without the use of magnetic fields. From optical measurements we extract the value of the interaction strength over the transition energy as high as g/ω ~ 0.55, deep in the USC regime, while the nanorod array occupies only ∼4% of the cavity volume. Moreover, by comparing the resonant energies of the coupled and uncoupled systems, we indirectly observe up to ∼10% modification of the ground-state energy, which is a hallmark of USC. Our results suggest that plasmon-microcavity polaritons are a promising platform for room-temperature USC realizations in the optical and infrared ranges, and may lead to the long-sought direct visualization of the vacuum energy modification.

Electrical Control of Hybrid Monolayer Tungsten Disulfide-Plasmonic Nanoantenna Light-Matter States at Cryogenic and Room Temperatures.

Hybrid light-matter states-polaritons-have attracted considerable scientific interest recently, motivated by their potential for development of nonlinear and quantum optical schemes. To realize such states, monolayer transition metal dichalcogenides (TMDCs) have been widely employed as excitonic materials. In addition to neutral excitons, TMDCs host charged excitons, which enables active tuning of hybrid light-matter states by electrical means. Although several reports demonstrated charged exciton-polaritons in various systems, the full-range interaction control attainable at room temperature has not been realized. Here, we demonstrate electrically tunable charged exciton-plasmon polaritons in a hybrid tungsten disulfide (WS2) monolayer-plasmonic nanoantenna system. We show that electrical gating of monolayer WS2 allows tuning the oscillator strengths of neutral and charged excitons not only at cryogenic but also at room temperature, both at vacuum and atmospheric pressure. Such electrical control enables a full-range tunable switching from strong neutral exciton-plasmon coupling to strong charged exciton-plasmon coupling. Our experimental findings allow discussing beneficial and limiting factors of charged exciton-plasmon polaritons, as well as offer routes toward realization of charged polaritonic devices at ambient conditions.

Collective Strong Light-Matter Coupling in Hierarchical Microcavity-Plasmon-Exciton Systems.

Polaritons are compositional light-matter quasiparticles that arise as a result of strong coupling between the vacuum field of a resonant optical cavity and electronic excitations in quantum emitters. Reaching such a regime is often hard, as it requires materials possessing high oscillator strengths to interact with the relevant optical mode. Two-dimensional transition metal dichalcogenides (TMDCs) have recently emerged as promising candidates for realization of strong coupling regime at room temperature. However, these materials typically provide coupling strengths in the range of 10-40 meV, which may be insufficient for reaching strong coupling with low quality factor resonators. Here, we demonstrate a universal scheme that allows a straightforward realization of strong coupling with 2D materials and beyond. By intermixing plasmonic excitations in nanoparticle arrays with excitons in a WS2 monolayer inside a resonant metallic microcavity, we fabricate a hierarchical system with the collective microcavity-plasmon-exciton Rabi splitting exceeding ∼500 meV at room temperature. Photoluminescence measurements of the coupled systems show dominant emission from the lower polariton branch, indicating the participation of excitons in the coupling process. Strong coupling has been recently suggested to affect numerous optical- and material-related properties including chemical reactivity, exciton transport, and optical nonlinearities. With the universal scheme presented here, strong coupling across a wide spectral range is within easy reach and therefore exploration of these exciting phenomena can be further pursued in a much broader class of materials.

Hyperlensing at NIR frequencies using a hemispherical metallic nanowire lens in a sea-urchin geometry.

Label-free and real time far-field super-resolution imaging (hyperlensing) at the nanoscale is of significant interest where sub-λ imaging remains a constraint because of Abbe's diffraction limit. Though by utilizing anisotropic permittivities, metal-dielectric multilayers have been successful in reconstructing high-frequency components of sub-λ objects, yet they remain cumbersome and expensive to make. Most of the multilayer structures require multiple vacuum deposition cycles and are plagued by stringent requirements on the surface roughness of metallic layers. In contrast to the multilayer structure here we propose a 3D hyperbolic metamaterial model composed of metallic nanorods arranged in a sea-urchin geometry as a hyper-lensing device, which is capable of projecting and magnifying diffraction limited information into the far-field at Near-infrared (NIR) frequencies. The hyperlens generates a band of flat hyperbolic dispersions in spherical coordinates, which in turn supports the propagation of high wave-vector spatial harmonics leading to far-field super-resolution imaging. Using full-wave finite-difference time-domain (FDTD) simulations with diffraction limited trimer, quadrumer and ringed objects etched on thin perfect electric conductor (PEC) films, we show that the hyperlens model can achieve magnification factors of up to 10× in the far-field (∼4.5λ from the object's surface) under a light source with a wavelength of 1 µm, with successful resolution down to 220 nm (∼λ/5). The magnified image field distribution projected into the far-field is shown to follow the object under a reduction in the symmetry. These results are important for making progress in the realization of real-time biomolecular imaging systems, eliminating the need for near-field scanning, destructive electron microscopy and various image post-processing techniques.

Engineering interfacial photo-induced charge transfer based on nanobamboo array architecture for efficient solar-to-chemical energy conversion.

Engineering interfacial photo-induced charge transfer for highly synergistic photocatalysis is successfully realized based on nanobamboo array architecture. Programmable assemblies of various components and heterogeneous interfaces, and, in turn, engineering of the energy band structure along the charge transport pathways, play a critical role in generating excellent synergistic effects of multiple components for promoting photocatalytic efficiency.