Self-Hybridized Vibrational-Mie Polaritons in Water Droplets.

We study the self-hybridization between Mie modes supported by water droplets with stretching and bending vibrations in water molecules. Droplets with radii >2.7  μm are found to be polaritonic on the onset of the ultrastrong light-matter coupling regime.

Quantum trapping and rotational self-alignment in triangular Casimir microcavities.

Casimir torque, a rotational motion driven by zero-point energy minimization, is a problem that attracts notable research interest. Recently, it has been realized using liquid crystal phases and natural anisotropic substrates. However, for natural materials, substantial torque occurs only at van der Waals distances of ~10 nm.

Probing optical anapoles with fast electron beams.

Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far.

Polaritonic linewidth asymmetry in the strong and ultrastrong coupling regime.

The intriguing properties of polaritons resulting from strong and ultrastrong light-matter coupling have been extensively investigated. However, most research has focused on spectroscopic characteristics of polaritons, such as their eigenfrequencies and Rabi splitting. Here, we study the decay rates of a plasmon-microcavity system in the strong and ultrastrong coupling regimes experimentally and numerically.

The Rise and Current Status of Polaritonic Photochemistry and Photophysics.

The interaction between molecular electronic transitions and electromagnetic fields can be enlarged to the point where distinct hybrid light-matter states, polaritons, emerge. The photonic contribution to these states results in increased complexity as well as an opening to modify the photophysics and photochemistry beyond what normally can be seen in organic molecules. It is today evident that polaritons offer opportunities for molecular photochemistry and photophysics, which has caused an ever-rising interest in the field.

Perfect Absorption and Strong Coupling in Supported MoS Multilayers.

Perfect absorption and strong coupling are two highly sought-after regimes of light-matter interactions. Both regimes have been studied as separate phenomena in excitonic 2D materials, particularly in MoS. However, the structures used to reach these regimes often require intricate nanofabrication.

Optical Constants of Several Multilayer Transition Metal Dichalcogenides Measured by Spectroscopic Ellipsometry in the 300-1700 nm Range: High Index, Anisotropy, and Hyperbolicity.

Transition metal dichalcogenides (TMDs) attract significant attention due to their remarkable optical and excitonic properties. It was understood already in the 1960s and recently rediscovered that many TMDs possess a high refractive index and optical anisotropy, which make them attractive for nanophotonic applications. However, accurate analysis and predictions of nanooptical phenomena require knowledge of dielectric constants along both in- and out-of-plane directions and over a broad spectral range, information that is often inaccessible or incomplete.

Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study.

Ultrastrong coupling (USC) is a distinct regime of light-matter interaction in which the coupling strength is comparable to the resonance energy of the cavity or emitter. In the USC regime, common approximations to quantum optical Hamiltonians, such as the rotating wave approximation, break down as the ground state of the coupled system gains photonic character due to admixing of vacuum states with higher excited states, leading to ground-state energy changes. USC is usually achieved by collective coherent coupling of many quantum emitters to a single mode cavity, whereas USC with a single molecule remains challenging.

Tunable self-assembled Casimir microcavities and polaritons.

Spontaneous formation of ordered structures-self-assembly-is ubiquitous in nature and observed on different length scales, ranging from atomic and molecular systems to micrometre-scale objects and living matter. Self-ordering in molecular and biological systems typically involves short-range hydrophobic and van der Waals interactions. Here we introduce an approach to micrometre-scale self-assembly based on the joint action of attractive Casimir and repulsive electrostatic forces arising between charged metallic nanoflakes in an aqueous solution.

Giant optical anisotropy in transition metal dichalcogenides for next-generation photonics.

Large optical anisotropy observed in a broad spectral range is of paramount importance for efficient light manipulation in countless devices. Although a giant anisotropy has been recently observed in the mid-infrared wavelength range, for visible and near-infrared spectral intervals, the problem remains acute with the highest reported birefringence values of 0.8 in BaTiS and h-BN crystals.

Enhancing Vibrational Light-Matter Coupling Strength beyond the Molecular Concentration Limit Using Plasmonic Arrays.

Vibrational strong coupling is emerging as a promising tool to modify molecular properties by making use of hybrid light-matter states known as polaritons. Fabry-Perot cavities filled with organic molecules are typically used, and the molecular concentration limits the maximum reachable coupling strength. Developing methods to increase the coupling strength beyond the molecular concentration limit are highly desirable.

Abundance of cavity-free polaritonic states in resonant materials and nanostructures.

Strong coupling between various kinds of material excitations and optical modes has recently shown potential to modify chemical reaction rates in both excited and ground states. The ground-state modification in chemical reaction rates has usually been reported by coupling a vibrational mode of an organic molecule to the vacuum field of an external optical cavity, such as a planar Fabry-Pérot microcavity made of two metallic mirrors. However, using an external cavity to form polaritonic states might (i) limit the scope of possible applications of such systems and (ii) might be unnecessary.

Room-Temperature Lasing from Mie-Resonant Nonplasmonic Nanoparticles.

Subwavelength particles supporting Mie resonances underpin a strategy in nanophotonics for efficient control and manipulation of light by employing both an electric and a magnetic optically induced multipolar resonant response. Here, we demonstrate that monolithic dielectric nanoparticles made of CsPbBr halide perovskites can exhibit both efficient Mie-resonant lasing and structural coloring in the visible and near-IR frequency ranges. We employ a simple chemical synthesis with nearly epitaxial quality for fabricating subwavelength cubes with high optical gain and demonstrate single-mode lasing governed by the Mie resonances from nanocubes as small as 310 nm by the side length.

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.

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.

Visualizing Spatial Variations of Plasmon-Exciton Polaritons at the Nanoscale Using Electron Microscopy.

Polaritons are compositional light-matter quasiparticles that have enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Recently, plasmon-exciton polaritons (plexcitons) have been realized in hybrid material systems composed of transition metal dichalcogenide (TMDC) materials and metal nanoparticles, expanding polaritonic concepts to room temperature and nanoscale systems that also benefit from the exotic properties of TMDC materials. Despite the enormous progress in understanding TMDC-based plexcitons using optical-based methods, experimental evidence of plexcitons formation has remained indirect and mapping their nanometer-scale characteristics has remained an open challenge.

Present and Future of Surface-Enhanced Raman Scattering.

The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products.

Strong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling.

Strong light-matter interactions in both the single-emitter and collective strong coupling regimes attract significant attention due to emerging applications in quantum and nonlinear optics as well as opportunities for modifying material-related properties. Exploration of these phenomena is theoretically demanding, as polaritons exist at the intersection between quantum optics, solid state physics, and quantum chemistry. Fortunately, nanoscale polaritons can be realized in small plasmon-molecule systems, enabling treatment with ab initio methods.

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.

Strong Light-Matter Coupling between Plasmons in Individual Gold Bi-pyramids and Excitons in Mono- and Multilayer WSe.

Monolayer transition-metal dichalcogenides (TMDCs) have attracted a lot of research attention recently, motivated by their remarkable optical properties and potential for strong light-matter interactions. Realization of strong plasmon-exciton coupling is especially desirable in this context because it holds promise for the enabling of room-temperature quantum and nonlinear optical applications. These efforts naturally require investigations at a single-nanoantenna level, which, in turn, should possess a compact optical mode interacting with a small amount of excitonic material.

Tunable Hybrid Fano Resonances in Halide Perovskite Nanoparticles.

Halide perovskites are known to support excitons at room temperatures with high quantum yield of luminescence that make them attractive for all-dielectric resonant nanophotonics and meta-optics. Here we report the observation of broadly tunable Fano resonances in halide perovskite nanoparticles originating from the coupling of excitons to the Mie resonances excited in the nanoparticles. Signatures of the photon-exciton (" hybrid") Fano resonances are observed in dark-field spectra of isolated nanoparticles, and also in the extinction spectra of aperiodic lattices of such nanoparticles.