2D Silver-Nanoplatelets Metasurface for Bright Directional Photoluminescence, Designed with the Local Kirchhoff's Law.

Semiconductor colloidal nanocrystals are excellent light emitters in terms of efficiency and spectral control. They can be integrated with a metasurface to make ultrathin photoluminescent devices with a reduced amount of active material and perform complex functionalities such as beam shaping or polarization control. To design such a metasurface, a quantitative model of the emitted power is needed. Here, we report the design, fabrication, and characterization of a ∼300 nm thick light-emitting device combining a plasmonic metasurface with an ensemble of nanoplatelets. The source has been designed with a methodology based on a local form of Kirchhoff's law. The source displays record high directionality and absorptivity.

Ultrasmall and tunable TeraHertz surface plasmon cavities at the ultimate plasmonic limit.

The ability to confine THz photons inside deep-subwavelength cavities promises a transformative impact for THz light engineering with metamaterials and for realizing ultrastrong light-matter coupling at the single emitter level. To that end, the most successful approach taken so far has relied on cavity architectures based on metals, for their ability to constrain the spread of electromagnetic fields and tailor geometrically their resonant behavior. Here, we experimentally demonstrate a comparatively high level of confinement by exploiting a plasmonic mechanism based on localized THz surface plasmon modes in bulk semiconductors. We achieve plasmonic confinement at around 1 THz into record breaking small footprint THz cavities exhibiting mode volumes as low as [Formula: see text], excellent coupling efficiencies and a large frequency tunability with temperature. Notably, we find that plasmonic-based THz cavities can operate until the emergence of electromagnetic nonlocality and Landau damping, which together constitute a fundamental limit to plasmonic confinement. This work discloses nonlocal plasmonic phenomena at unprecedentedly low frequencies and large spatial scales and opens the door to novel types of ultrastrong light-matter interaction experiments thanks to the plasmonic tunability.

Over-coupled resonator for broadband surface enhanced infrared absorption (SEIRA).

Detection of molecules is a key issue for many applications. Surface enhanced infrared absorption (SEIRA) uses arrays of resonant nanoantennas with good quality factors which can be used to locally enhance the illumination of molecules. The technique has proved to be an effective tool to detect small amount of material. However, nanoresonators can detect molecules on a narrow bandwidth so that a set of resonators is necessary to identify a molecule fingerprint. Here, we introduce an alternative paradigm and use low quality factor resonators with large radiative losses (over-coupled resonators). The bandwidth enables to detect all absorption lines between 5 and 10 µm, reproducing the molecular absorption spectrum. Counterintuitively, despite a lower quality factor, the system sensitivity is improved and we report a reflectivity variation as large as one percent per nanometer of molecular layer of PMMA. This paves the way to specific identification of molecules. We illustrate the potential of the technique with the detection of the explosive precursor 2,4-dinitrotoluene (DNT). There is a fair agreement with electromagnetic simulations and we also introduce an analytic model of the SEIRA signal obtained in the over-coupling regime.

Controlling light emission by a thermalized ensemble of colloidal quantum dots with a metasurface.

We report an experimental and theoretical study of light emission by a patterned ensemble of colloidal quantum dots (cQDs). This system modifies drastically the emission spectrum and polarization as compared to a planar layer of cQDs. It exhibits bright, directional and polarized emission including a degree of circular polarization in some directions. We introduce a model of light emission based on a local Kirchhoff law which reproduces accurately all the features of the experiment. The model provides a figure of merit to assess quantitatively the emitted power. This work paves the way to the systematic design of efficient ultrathin light emitting metasurfaces with controlled polarization, spectrum and directivity.

Dispersion-based intertwined SEIRA and SPR effect detection of 2,4-dinitrotoluene using a plasmonic metasurface.

Surface enhanced infrared absorption (SEIRA) spectroscopy and surface plasmon resonance (SPR) make possible, thanks to plasmonics nanoantennas, the detection of low quantities of biological and chemical materials. Here, we investigate the infrared response of 2,4-dinitrotoluene deposited on various arrays of closely arranged metal-insulator-metal (MIM) resonators and experimentally show how the natural dispersion of the complex refractive index leads to an intertwined combination of SEIRA and SPR effect that can be leveraged to identify molecules. They are shown to be efficient for SEIRA spectroscopy and allows detecting of the dispersive explosive material, 2,4-dinitrotoluene. By changing the in-plane parameters, a whole spectral range of absorptions of 2,4-DNT is scanned. These results open the way to the design of sensors based on SEIRA and SPR combined effects, without including a spectrometer.

Far-field excitation of single graphene plasmon cavities with ultracompressed mode volumes.

Acoustic graphene plasmons are highly confined electromagnetic modes carrying large momentum and low loss in the mid-infrared and terahertz spectra. However, until now they have been restricted to micrometer-scale areas, reducing their confinement potential by several orders of magnitude. Using a graphene-based magnetic resonator, we realized single, nanometer-scale acoustic graphene plasmon cavities, reaching mode volume confinement factors of ~5 × 1010 Such a cavity acts as a mid-infrared nanoantenna, which is efficiently excited from the far field and is electrically tunable over an extremely large broadband spectrum. Our approach provides a platform for studying ultrastrong-coupling phenomena, such as chemical manipulation via vibrational strong coupling, as well as a path to efficient detectors and sensors operating in this long-wavelength spectral range.

Global polarizability matrix method for efficient modeling of light scattering by dense ensembles of non-spherical particles in stratified media.

We introduce a numerical method that enables efficient modeling of light scattering by large, disordered ensembles of non-spherical particles incorporated in stratified media, including when the particles are in close vicinity to each other, to planar interfaces, and/or to localized light sources. The method consists of finding a small set of fictitious polarizable elements-or numerical dipoles-that quantitatively reproduces the field scattered by an individual particle for any excitation and at an arbitrary distance from the particle surface. The set of numerical dipoles is described by a global polarizability matrix that is determined numerically by solving an inverse problem relying on fullwave simulations. The latter are classical and may be performed with any Maxwell's equations solver. Spatial non-locality is an important feature of the numerical dipoles set, providing additional degrees of freedom compared to classical coupled dipoles to reconstruct complex scattered fields. Once the polarizability matrix describing scattering by an individual particle is determined, the multiple scattering problem by ensembles of such particles in stratified media can be solved using a Green tensor formalism and only a few numerical dipoles, thereby with a low physical memory usage, even for dense systems in close vicinity to interfaces. The performance of the method is studied with the example of large high-aspect-ratio high-index dielectric cylinders. The method is easy to implement and may offer new possibilities for the study of complex nanostructured surfaces, which are becoming widespread in emerging photonic technologies.

Extreme multiexciton emission from deterministically assembled single-emitter subwavelength plasmonic patch antennas.

Coupling nano-emitters to plasmonic antennas is a key milestone for the development of nanoscale quantum light sources. One challenge, however, is the precise nanoscale positioning of the emitter in the structure. Here, we present a laser etching protocol that deterministically positions a single colloidal CdSe/CdS core/shell quantum dot emitter inside a subwavelength plasmonic patch antenna with three-dimensional nanoscale control. By exploiting the properties of metal-insulator-metal structures at the nanoscale, the fabricated single-emitter antenna exhibits a very high-Purcell factor (>72) and a brightness enhancement of a factor of 70. Due to the unprecedented quenching of Auger processes and the strong acceleration of the multiexciton emission, more than 4 photons per pulse can be emitted by a single quantum dot, thus increasing the device yield. Our technology can be applied to a wide range of photonic nanostructures and emitters, paving the way for scalable and reliable fabrication of ultra-compact light sources.

Antenna surface plasmon emission by inelastic tunneling.

Surface plasmons polaritons are mixed electronic and electromagnetic waves. They have become a workhorse of nanophotonics because plasmonic modes can be confined in space at the nanometer scale and in time at the 10 fs scale. However, in practice, plasmonic modes are often excited using diffraction-limited beams. In order to take full advantage of their potential for sensing and information technology, it is necessary to develop a microscale ultrafast electrical source of surface plasmons. Here, we report the design, fabrication and characterization of nanoantennas to emit surface plasmons by inelastic electron tunneling. The antenna controls the emission spectrum, the emission polarization, and enhances the emission efficiency by more than three orders of magnitude. We introduce a theoretical model of the antenna in good agreement with the results.

Quasi-confined ENZ mode in an anisotropic uniaxial thin slab.

In this paper, we present a numerical modal study of a simple slab, made of an uniaxial anisotropic material having an "epsilon-near-zero" (ENZ) dielectric function, surrounded by vacuum. We use two Drude models with a different plasma frequency for the direction parallel and perpendicular to the slab surface as toy models to study the effect of uniaxial anisotropy of type I (∊‖ > 0, ∊⊥ < 0) and type II (∊‖ < 0, ∊⊥ > 0) on the different electromagnetic modes of the system. In addition to the so-called ENZ mode, studied in detail by Campione et. al [ Phys. Rev. B91, 121408(R) (2015)], the slab can support quasi-confined (QC) mode in the type I and type II anisotropy frequency ranges. We show that those modes exhibit a strong electric field enhancement, caused by the ENZ character of the dielectric function. In strong contrast with the ENZ mode, QC modes can have a strong electric field enhancement for thick slabs, with a Fabry-Perot-like electromagnetic field distribution spanning over the whole slab thickness. This opens the way for large electric field enhancement in thick slabs with QC ENZ modes. Thick slabs also allow metamaterial designs, giving the possibility to engineer the anisotropy of the effective dielectric function, opening interesting perspectives for the control of field enhancement of the ENZ QC modes and their integration in operating devices, such as detectors, sources, or modulators.

Directional light beams by design from electrically driven elliptical slit antennas.

We report on the low-energy, electrical generation of light beams in specific directions from planar elliptical microstructures. The emission direction of the beam is determined by the microstructure eccentricity. A very simple, broadband, optical antenna design is used, which consists of a single elliptical slit etched into a gold film. The light beam source is driven by an electrical nanosource of surface plasmon polaritons (SPP) that is located at one focus of the ellipse. In this study, SPPs are generated through inelastic electron tunneling between a gold surface and the tip of a scanning tunneling microscope.

True thermal antenna with hyperbolic metamaterials.

A thermal antenna is an electromagnetic source that emits in its surrounding a spatially coherent field in the infrared frequency range. Usually, its emission pattern changes with the wavelength so that the heat flux it radiates is weakly directive. Here, we show that a class of hyperbolic materials of type II possess a Brewster angle, which is weakly dependent on the wavelength, so that they can radiate like a true thermal antenna with a highly directional and p-polarized heat flux. The realization of these sources could open a new avenue in the field of thermal management in far-field regime.

Anti-coalescence of bosons on a lossy beam splitter.

Two-boson interference, a fundamentally quantum effect, has been extensively studied with photons through the Hong-Ou-Mandel effect and observed with guided plasmons. Using two freely propagating surface plasmon polaritons (SPPs) interfering on a lossy beam splitter, we show that the presence of loss enables us to modify the reflection and transmission factors of the beam splitter, thus revealing quantum interference paths that do not exist in a lossless configuration. We investigate the two-plasmon interference on beam splitters with different sets of reflection and transmission factors. Through coincidence-detection measurements, we observe either coalescence or anti-coalescence of SPPs. The results show that losses can be viewed as a degree of freedom to control quantum processes.

Directional and monochromatic thermal emitter from epsilon-near-zero conditions in semiconductor hyperbolic metamaterials.

The development of novel thermal sources that control the emission spectrum and the angular emission pattern is of fundamental importance. In this paper, we investigate the thermal emission properties of semiconductor hyperbolic metamaterials (SHMs). Our structure does not require the use of any periodic corrugation to provide monochromatic and directional emission properties. We show that these properties arise because of epsilon-near-zero conditions in SHMs. The thermal emission is dominated by the epsilon-near-zero effect in the doped quantum wells composing the SHM. Furthermore, different properties are observed for s and p polarizations, following the characteristics of the strong anisotropy of hyperbolic metamaterials.

Nanoantenna for Electrical Generation of Surface Plasmon Polaritons.

Light emission by inelastic tunneling has been known for many years. Recently, this technique has been used to generate surface plasmons using a scanning tunneling microscope tip. The emission process suffers from a very low efficiency lower than a photon in 10^{4} electrons. We introduce a resonant plasmonic nanoantenna that allows both enhancing the power conversion to surface plasmon polaritons by more than 2 orders of magnitude and narrowing the emission spectrum. The physics of the emission process is analyzed in terms of local density of states and the efficiency of the nanoantenna to radiate surface plasmon polaritons.

Single-plasmon interferences.

Surface plasmon polaritons are electromagnetic waves coupled to collective electron oscillations propagating along metal-dielectric interfaces, exhibiting a bosonic character. Recent experiments involving surface plasmons guided by wires or stripes allowed the reproduction of quantum optics effects, such as antibunching with a single surface plasmon state, coalescence with a two-plasmon state, conservation of squeezing, or entanglement through plasmonic channels. We report the first direct demonstration of the wave-particle duality for a single surface plasmon freely propagating along a planar metal-air interface. We develop a platform that enables two complementary experiments, one revealing the particle behavior of the single-plasmon state through antibunching, and the other one where the interferences prove its wave nature. This result opens up new ways to exploit quantum conversion effects between different bosonic species as shown here with photons and polaritons.

Non-blinking quantum dot with a plasmonic nanoshell resonator.

Colloidal semiconductor quantum dots are fluorescent nanocrystals exhibiting exceptional optical properties, but their emission intensity strongly depends on their charging state and local environment. This leads to blinking at the single-particle level or even complete fluorescence quenching, and limits the applications of quantum dots as fluorescent particles. Here, we show that a single quantum dot encapsulated in a silica shell coated with a continuous gold nanoshell provides a system with a stable and Poissonian emission at room temperature that is preserved regardless of drastic changes in the local environment. This novel hybrid quantum dot/silica/gold structure behaves as a plasmonic resonator with a strong Purcell factor, in very good agreement with simulations. The gold nanoshell also acts as a shield that protects the quantum dot fluorescence and enhances its resistance to high-power photoexcitation or high-energy electron beams. This plasmonic fluorescent resonator opens the way to a new family of plasmonic nanoemitters with robust optical properties.

Aperiodic-Fourier modal method for analysis of body-of-revolution photonic structures.

Modeling the field produced by a point-like dipole with an arbitrary location in the presence of a rotationally invariant nanostructure is an important issue in the context of designing nanoantennas. This is a challenging problem, as rotational symmetry is broken when introducing a noncentered dipole. Antennas larger than the wavelength are required for directivity, whereas the dipole-antenna distance is highly subwavelength, so there are two different length scales in the problem. In this paper, we introduce an original S-matrix approach based on an aperiodic-Fourier modal method. The potential of the technique is illustrated by considering three examples. We compare our results with a finite element technique.

Cooperative electromagnetic interactions between nanoparticles for solar energy harvesting.

The cooperative electromagnetic interactions between discrete resonators have been widely used to modify the optical properties of metamaterials. Here we propose a general approach for engineering these interactions both in the dipolar approximation and for any higher-order description. Finally we apply this strategy to design broadband absorbers in the visible range from simple n-ary arrays of metallic nanoparticles.

Stimulated emission depletion microscopy resolves individual nitrogen vacancy centers in diamond nanocrystals.

Nitrogen-vacancy (NV) color centers in nanodiamonds are highly promising for bioimaging and sensing. However, resolving individual NV centers within nanodiamond particles and the controlled addressing and readout of their spin state has remained a major challenge. Spatially stochastic super-resolution techniques cannot provide this capability in principle, whereas coordinate-controlled super-resolution imaging methods, like stimulated emission depletion (STED) microscopy, have been predicted to fail in nanodiamonds. Here we show that, contrary to these predictions, STED can resolve single NV centers in 40-250 nm sized nanodiamonds with a resolution of ≈10 nm. Even multiple adjacent NVs located in single nanodiamonds can be imaged individually down to relative distances of ≈15 nm. Far-field optical super-resolution of NVs inside nanodiamonds is highly relevant for bioimaging applications of these fluorescent nanolabels. The targeted addressing and readout of individual NV(-) spins inside nanodiamonds by STED should also be of high significance for quantum sensing and information applications.