We present an analytical approach to the calculation of the linewidth and lineshift of an atom or molecule in the near field of a structured dielectric surface. For soft surface corrugations with amplitude lambda/50, we find variations of the linewidth in the ten percent region. More strikingly, the shift of the molecular resonance can reach several natural linewidths. We demonstrate that the lateral resolution is of the order of the molecule-surface distance. We give a semiquantitative explanation of the outcome of our calculations that is based on simple intuitive models.
Plasmonic structures interacting with light provide electromagnetic resonances which result in a high degree of local field confinement enabling the enhancement of light-matter interaction. Plasmonic structures typically consist of metals which, however, suffer from very high ohmic losses and heating. High-index dielectrics, on the other hand, can serve as an alternative material due to their low-dissipative nature and strong scattering abilities. We study the optical properties of a system composed of all-dielectric nanoparticle arrays covered with a film of organic dye molecules (IR-792), an…
Metasurfaces are nano-structured devices composed of arrays of subwavelength scatterers (or meta-atoms) that manipulate the wavefront, polarization, or intensity of light. Like other diffractive optical devices, metasurfaces suffer from significant chromatic aberrations that limit their bandwidth. Here, we present a method for designing multiwavelength metasurfaces using unit cells with multiple meta-atoms, or meta-molecules. Transmissive lenses with efficiencies as high as 72% and numerical apertures as high as 0.46 simultaneously operating at 915 nm and 1550 nm are demonstrated. With proper …
We report strong coupling of a monolayer of J-aggregated dye molecules to the whispering gallery modes of a dielectric microsphere at room temperature. We systematically studied the evolution of strong coupling as the number of layers of dye molecules was increased, we found the Rabi splitting to rise from 56 meV for a single layer to 94 meV for four layers of dye molecules. We compare our experimental results with 2D numerical simulations and a simple coupled oscillator model, finding good agreement. We anticipate that these results will act as a stepping stone for integrating molecule-cavity…
Plasmonic nanoantennas, the properties of which are essentially determined by their resonance modes, are of interest both fundamentally and for various applications. Antennas with various shapes, geometries and compositions have been demonstrated, each possessing unique properties and potential applications. Here, we propose the use of a sidewall coating as an additional degree of freedom to manipulate plasmonic gap cavity modes in strongly coupled metallic nanodisks. It is demonstrated that for a dielectric middle layer with a thickness of a few tens of nanometers and a sidewall plasmonic coa…
We demonstrate an enhanced emission of high quantum yield molecules coupled to dielectric metasurfaces formed by periodic arrays of polycrystalline silicon nanoparticles. Radiative coupling of the nanoparticles, mediated by in-plane diffraction, leads to the formation of collective Mie scattering resonances or Mie surface lattice resonances (M-SLRs), with remarkable narrow line widths. These narrow line widths and the intrinsic electric and magnetic dipole moments of the individual Si nanoparticles allow to resolve electric and magnetic M-SLRs. Incidence angle- and polarization-dependent extin…
Light confinement induced by resonant states in aperiodic photonic structures are interesting for many applications. A particular case of these resonances can be found in 2D quasi-crystalline arrangements of dielectric cylinders. These systems present a rather isotropic band gap as well as isolated in-gap photonic states (as a result of spatially localized resonances). These states are built by high symmetry polygonal clusters that can be regarded as photonic molecules. In this paper we study the transmission properties of a slab of glass cylinders arranged in approximants of decagonal quasi-c…
These notes, intended to be self contained and tutorial, present a direct, macroscopic approach to quantizing light inside a linear-response dielectric material when both spectral dispersion and spatial nonuniformity are present, but the spectral region of interest is optically transparent so that explicit treatment of the underlying physics of the medium is not needed. The approach taken is based on the macroscopic Maxwell equations and a corresponding Hamiltonian, without the use of Lagrangians or any dynamical model for the medium, and uses a standard mode-based quantization method. The tre…
We present a novel differential refractive index sensor based on arrays of photonic molecules (PM) of dielectric cylinders and two structural defect cavities. The transmission spectrum of the photonic proposed structure as sensor shows a wide photonic stop band with two localized states. One of them, the reference state, is bound to a decagonal ring of cylinders and the other, the sensing state, to the defect cavities of the lattice. It is shown that defect mode is very sensitive to the presence of materials with dielectric permittivity different from that of the surrounding cylinders while th…
Localization of single fluorescent molecules is key for physicochemical and biophysical measurements such as single-molecule tracking and super-resolution imaging by single-molecule localization microscopy (SMLM). Recently a series of methods have been developed in which the localization precision is enhanced by interrogating the molecular position with a sequence of spatially modulated patterns of light. Among them, the MINFLUX technique outstands for achieving a ~10-fold improvement compared to wide-field camera-based single-molecule localization, reaching ~1-2 nm localization precision at m…
Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk array…
We introduce transversely structured all-dielectric waveguides which exploit the vectorial nature of light to achieve extreme sub-wavelength confinement in high index dielectrics, enabling characteristic mode dimensions below $λ_0^2$/1,000 without metals or plasmonics. We also derive the metric of optical concentration and show its convenient usage in characterizing enhanced linear and non-linear interactions at the nanoscale. This work expands the toolbox of nanophotonics and opens the door to new types of ultra-efficient and record performing linear and nonlinear devices with broad applicati…
Photonic components based on structured metallic elements show great potential for device applications where field enhancement and confinement of the radiation on a subwavelength scale is required. In this paper we report a detailed study of a prototypical metallo-dielectric photonic structure, where features well known in the world of dielectric photonic crystals, like band gaps and defect modes, are exported to the metallic counterpart, with interesting applications to infrared science and technology, as for instance in quantum well infrared photodetectors, narrow-band spectral filters, and …
We propose a coherent optical method for creating negative refractive index (NRI) for a gaseous ensemble of ground-state polar molecules possessing both permanent electric and magnetic moments. Exploiting the pure rotational transition between the two lowest rotational levels of the ground vibrational state one can generate two dressed states of mixed parity using a microwave laser. These dressed states are then used as the two lower states of a Λ-type three-level scheme using two infrared lasers to couple them to another ro-vibrational level in the ground-state manifold. One of the infrared l…
Optomechanical arrays made of structured flexible dielectrics are a promising system for exploring quantum and many-body optomechanical phenomena. We generalize investigations of the optomechanical properties of periodic arrays of one-dimensional scatterers in optical resonators to the case of vibrating membranes whose thickness is not necessarily small with respect to the optical wavelength of interest. The array optical transmission spectrum and its optomechanical coupling with a linear Fabry-Perot cavity field are investigated both analytically and numerically.
We demonstrated remote plasmonic enhancement (RPE) by a dense random array of Ag nanoislands (AgNIs) that were partially gold-alloyed and attached with column-structured silica (CSS) overlayer of more than 100 nm in thickness. The physical and chemical protection of the CSS layer could lead to reducing the mutual impact between analyte molecules and metal nanostructures. RPE plate was realized just by sputtering and chemical immersion processes, resulting in high productivity. We found a significant enhancement on the order of 10$^7$-fold for Raman scattering and 10$^2$-fold for fluorescence b…
A very efficient method for the calculation of the effective optical response of nano-structured composite systems allows the design of metamaterials tailored for specific optical polarization properties. We use our method to design 2D periodic arrays of sub-wavelength dielectric inclusions within nanometric supported metallic thin films which behave as either an almost perfect linearly dichroic system, as a controllable source of circular polarized light, as a system with a large circular dichroism, or as a circular polarizer. All of these systems may be tuned over a wide energy range.
Tremendous enhancement of light-matter interaction in plasmon-excited molecular hybrid devices allows for non-linearities on the level of single emitters and few photons. This promises a plethora of novel applications like single photon transistors. Nevertheless, building the components of such devices is technologically extremely challenging. We tackle this task by lithographically fabricating on-chip plasmonic waveguides, efficiently connected to far-field in- and out-coupling ports via low-loss dielectric waveguides. Furthermore, a nano-assembling technology is developed, enabling the contr…
From surface to volume plasmons in hyperbolic metamaterials: General existence conditions for bulk high-k waves in metal-dielectric and graphene-dielectric multilayers
We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order auto-correlation and cross-correlation functions show that the emitter is a single molecule and that the light emergi…
