Hyper-doped silicon nanoantennas and metasurfaces for tunable infrared plasmonics
Jean-Marie Poumirol, Clément Majorel, Nicolas Chery, Christian Girard, Peter R. Wiecha, Nicolas Mallet, Guilhem Larrieu, Fuccio Cristiano, Richard Monflier, Ann… 展开作者
Jean-Marie Poumirol, Clément Majorel, Nicolas Chery, Christian Girard, Peter R. Wiecha, Nicolas Mallet, Guilhem Larrieu, Fuccio Cristiano, Richard Monflier, Anne-Sophie Royet, Pablo Acosta Alba, Sébastien Kerdiles, Vincent Paillard, Caroline Bonafos
We present the experimental realization of ordered arrays of hyper-doped silicon nanodisks, which exhibit a localized surface plasmon resonance. The plasmon is widely tunable in a spectral window between 2 and 5 $μ$m by adjusting the free carrier concentration between 10$^{20}$ and 10$^{21}$ cm$^{-3}$. We show that strong infrared light absorption can be achieved with all-silicon plasmonic metasurfaces employing nano-structures with dimensions as low as 100\,nm in diameter and 23 nm in height. Our numerical simulations show an excellent agreement with the experimental data and provide physical insights on the impact of the nanostructure shape as well as of near-field effects on the optical properties of the metasurface. Our results open highly promising perspectives for integrated all-silicon-based plasmonic devices for instance for chemical or biological sensing or for thermal imaging.
Metasurfaces are ultrathin nanostructured surfaces that can allow arbitrary manipulation of light. Implementing dynamic tunability into their design could allow the optical functions of metasurfaces to be rapidly modified at will. The most pronounced and robust tunability of optical properties is provided by phase-change materials such as vanadium dioxide (VO2) and germanium antimony telluride (GST), but their implementations have been limited only to near-infrared wavelengths. Here, we demonstrate that VO2 nanoantennas with widely tunable Mie resonances can be utilized for designing tunable m…
A rigorous theory of photon emission accompanied inelastic tunnelling inside the gap of plasmonic nanoantennas has been developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. Resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven nanoplasmonic circuits.
We present a new design of plasmonic nanoantenna with a slant gap for optical chirality engineering. At resonance, the slant gap provides highly enhanced electric field parallel to external magnetic field with a phase delay of 90 degree, resulting in enhanced optical chirality. We show by numerical simulations that upon linearly polarized excitation our achiral nanoantenna can generate near field with enhanced optical chirality that can be tuned by the slant angle and resonance condition. Our design can be easily realized and may find applications in circular dichroism enhancement.
Boosting nonlinear frequency conversion in extremely confined volumes remains a key challenge in nano-optics, nanomedicine, photocatalysis, and background-free biosensing. To this aim, field enhancements in plasmonic nanostructures are often exploited to effectively compensate for the lack of phase-matching at the nanoscale. Second harmonic generation (SHG) is, however, strongly quenched by the high degree of symmetry in plasmonic materials at the atomic scale and in nanoantenna designs. Here, we devise a plasmonic nanoantenna lacking axial symmetry, which exhibits spatial and frequency mode o…
We present a novel procedure for manipulating the near-field of plasmonic nanoantennas using neural network-controlled laser pulse-shaping. As model systems we numerically studied the spatial distribution of the second harmonic response of L-shaped nanoantennas illuminated by broadband laser pulses. We first show that a trained neural network can be used to predict the relative intensity of the second-harmonic hotspots of the nanoantenna for a given spectral phase and that it can be employed to deterministically switch individual hotspots on and off on sub-diffraction length scale by shaping t…
We present a practical new method for fabricating a coupled single quantum emitter-plasmonic nanoantenna system. Emission characteristics of a single defect center embedded in hexagonal Boron Nitride (hBN) multilayers is modified using plasmonic nanoantennas. By dewetting thin silver films on hBN multilayers, plasmonic nanoantennas are obtained in a size controlled way with no adverse effects on the defects. A very same single defect center is investigated with and without nanoantenna in order to demonstrate the modification of its emission characteristics. Based on the initial silver film thi…
Plasmonic nanostructures that support surface plasmon (SP) resonance potentially provide a route for the development of nanoengineered nonlinear optical devices. In this work, second-order nonlinear light scattering, specifically sum-frequency generation (SFG) and second-harmonic generation (SHG), from plasmonic nanoantennas is modeled by the boundary element method (BEM). Far-field scattering patterns are compared with the results calculated by the Mie theory to validate the accuracy of the developed nonlinear solver. The SFG from a multi-resonant nanoantenna (MR-NA) and the SHG from a partic…
Freed from phase-matching constraints, plasmonic metasurfaces have contributed significantly to the control of the optical nonlinearity and enhancing the nonlinear generation efficiency by engineering subwavelength meta-atoms. However, the high dissipative losses and the inevitable thermal heating limit their applicability in nonlinear nanophotonics. All-dielectric metasurfaces, supporting both electric and magnetic Mie-type resonances in their nanostructures, have appeared as a promising alternative to nonlinear plasmonics. High-index dielectric nanostructures, allowing additional magnetic re…
Nanoantennas for light enhance light-matter interaction at the nanoscale making them useful in optical communication, sensing, and spectroscopy. So far nanoantenna engineering has been largely based on rules derived from the radio frequency domain which neglect the inertia of free metal electrons at optical frequencies causing phenomena such as complete field penetration, ohmic losses and plasmon resonances. Here we introduce a general and scalable evolutionary algorithm that accounts for topological constrains of the fabrication method and therefore yields unexpected nanoantenna designs exhib…
Electrically-driven optical antennas can serve as compact sources of electromagnetic radiation operating at optical frequencies. In the most widely explored configurations, the radiation is generated by electrons tunneling between metallic parts of the structure when a bias voltage is applied across the tunneling gap. Rather than relying on an inherently inefficient inelastic light emission in the gap, we suggest to use a ballistic nanoconstriction as the feed element of an optical antenna supporting plasmonic modes. We discuss the underlying mechanisms responsible for the optical emission, an…
The performance of plasmonic nanoantenna structures on top of SOI wire waveguides as coherent perfect absorbers for modulators and all-optical switches is explored. The absorption, scattering, reflection and transmission spectra of gold and aluminum nanoantenna-loaded waveguides were calculated by means of 3D finite-difference time-domain simulations for single waves propagating along the waveguide, as well as for standing wave scenarios composed from two counterpropagating waves. The investigated configurations showed losses of roughly 1% and extinction ratios greater than 25 dB for modulator…
The nonlinear process of second harmonic generation (SHG) in monolayer (1L) transition metal dichalcogenides (TMD), like $WS_2$, strongly depends on the polarization state of the excitation light. Combining plasmonic nanostructures with $1L-WS_2$ by transferring it onto a plasmonic nanoantenna array, a hybrid metasurface is realized impacting the polarization dependency of its SHG. Here, we investigate how plasmonic dipole resonances affect the process of SHG in plasmonic-TMD hybrid metasurfaces by nonlinear spectroscopy. We show, that the polarization dependency is affected by the lattice str…
Orbital angular momentum of light has recently been recognized as a new degree of freedom to encode information in quantum communication using light pulses. Methods to extract this information include reversing the process by which such twisted light was created in the first place or interference with other beams. Here, we propose an alternative new way to directly read out the extra information encoded in twisted light using plasmonic nanoantennas by con- verting the information about the orbital angular momentum of light into spectral information using bright and dark modes. Exemplarily cons…
Thermonanophotonics, i.e. the study of photothermal effects in optical nanoantennas, has recently attracted growing interest. While thermoplasmonic structures enable a broad range of applications, from imaging and optofluidics devices to medical and photochemical systems, dielectric nanoantennas open new opportunities for thermo-optical modulation and reconfigurable metasurfaces. However, computing both photo-thermal and thermo-optical effects in large arrays of nanoantennas remains a challenge. In this work, we implement a fast numerical method to compute the temperature increase of multi-dim…
Nanostructures of conventional metals offer manipulation of light at the nanoscale but are limited to static behavior due to their fixed material properties. To develop the next frontier of dynamic nanooptics and metasurfaces, we utilize the redox-tunable optical properties of conducting polymers, which were recently shown to be capable of sustaining plasmons in their most conducting oxidized state. Using nanodisks of poly(3,4-ethylenedioxythiophene:sulfate) (PEDOT:Sulf) as a model system, we present the first electrically tunable conducting polymer nanooptical antennas. In addition to repeate…
We present numerical studies, nano-fabrication and optical characterization of bowtie nanoantennas demonstrating their superior performance with respect to the electric field enhancement as compared to other Au nanoparticle shapes. For optimized parameters, we found mean intensity enhancement factors >2300x in the feed-gap of the antenna, decreasing to 1300x when introducing a 5nm titanium adhesion layer. Using electron beam lithography we fabricated gold bowties on various substrates with feed-gaps and tip radii as small as 10nm. In polarization resolved measurement we experimentally observed…
Plasmonic nanostructures attract tremendous attention as they confine electromagnetic fields well below the diffraction limit while simultaneously sustaining extreme local field enhancements. To fully exploit these properties, the identification and classification of resonances in such nanostructures is crucial. Recently, a novel figure of merit for resonance classification has been proposed 1 and its applicability was demonstrated mostly to toy model systems. This novel measure, the energy-based plasmonicity index (EPI), characterizes the nature of resonances in molecular nanostructures. The …
Metal nanostructures are key elements in nanooptics owing to their strong resonant interaction with light through local plasmonic charge oscillations. Their ability to shape light at the nanoscale have made them important across a multitude of areas, including biosensing, energy conversion and ultrathin flat metaoptics. Yet another dimension of avenues is foreseen for dynamic nanoantennas, ranging from tuneable metalenses for miniaturized medical devices to adaptable windows that control radiation flows in and out of buildings. However, enabling nano-optical antennas to be dynamically controll…
Coherent perfect absorption (CPA) describes the absence of all outgoing modes from a lossy resonator, driven by lossless incoming modes. Here, we show that for nanoresonators that also exhibit radiative losses, e.g. plasmonic nanoantennas, a generalized version of CPA (gCPA) can be applied. In gCPA outgoing modes are sup-pressed only for a subset of (guided plasmonic) modes while other (radiative) modes are treated as additional loss channels - a situation typically referred to as perfect impedance matching. Here we make use of gCPA to show how to achieve perfect impedance matching between a s…
Light localization is controlled at a scale of lambda/10 in the harmonic regime from the far field domain in a plasmonic nanoantenna. The nanoantenna under study consists of 3 aligned spheres 50 nm in diameter separated by a distance of 5 nm. By simply tuning the orientation of an incident plane wave, symmetric and antisymmetric mode-balancing induces a strong enhancement of the near field intensity in one cavity while nullifying the light intensity in the other cavity. Furthermore, it is demonstrated that the dipolar moment of a plasmonic particle can be fully extinguished when strongly coupl…
We demonstrate how the controlled positioning of a plasmonic nanoparticle modifies the photoluminescence of a single epitaxial GaAs quantum dot. The antenna particle leads to an increase of the luminescence intensity by about a factor of eight. Spectrally and temporally resolved photoluminescence measurements prove an increase of the quantum dot's excitation rate. The combination of stable epitaxial quantum emitters and plasmonic nanostructures promises to be highly beneficial for nanoscience and quantum optics.
We design a photonic sphere-array nanoantenna (NA) exhibiting both strong directionality and wavelength selectivity. Although the geometric configuration of the photonic NA resembles a plasmonic Yagi-Uda NA, it has different working principles, and most importantly, reduces the inherent metallic loss from plasmonic elements. For any selected optical wavelength, a sharp Fano-resonance by the reflector is tunable to overlap spectrally with a wider dipole resonance by the sphere-chain director leading to the high directionality. The work provides design principles for directional and selective ph…
Nanophotonic (nanoplasmonic) structures confine, guide, and concentrate light on the nanoscale. Advancement of nanophotonics critically depends on active nanoscale control of these phenomena. Localized control of the insulator and metallic phases of vanadium dioxide (VO2) would open up a universe of applications in nanophotonics via modulation of the local dielectric environment of nanophotonic structures allowing them to function as active devices. Here we show dynamic reversible control of VO2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantenn…
We present the simulation, fabrication and optical characterization of plasmonic gold bowtie nanoantennas on a semiconducting GaAs substrate as geometrical parameters such as size, feed gap, height and polarization of the incident light are varied. The surface plasmon resonance was probed using white light reflectivity on an array of nominally identical, 35nm thick Au antennas. To elucidate the influence of the semiconducting, high refractive index substrate, all experiments were compared using nominally identical structures on glass. Besides a linear shift of the surface plasmon resonance fro…
We review the latest theoretical advances in the application of the framework of Transformation Optics for the analytical description of deeply sub-wavelength electromagnetic phenomena. First, we present a general description of the technique, together with its usual exploitation for metamaterial conception and optimization in different areas of wave physics. Next, we discuss in detail the design of plasmonic metasurfaces, including the description of singular geometries which allow for broadband absorption in ultrathin platforms. Finally, we discuss the quasi-analytical treatment of plasmon-e…
The coupled light-matter modes supported by plasmonic metasurfaces can be combined with topological principles to yield subwavelength topological valley states of light. We give a systematic presentation of the topological valley states available for lattices of metallic nanoparticles: All possible lattices with hexagonal symmetry are considered, as well as valley states emerging on a square lattice. Several unique effects which have yet to be explored in plasmonics are identified, such as robust guiding, filtering and splitting of modes, as well as dual-band effects. We demonstrate these by m…
We investigate experimentally Third Harmonic Generation (THG) from plasmonic metasurfaces consisting of two-dimensional rectangular lattices of centrosymmetric gold nano-bars. By varying the incidence angle and the lattice period, we show how Surface Lattice Resonances (SLRs) at the involved wavelengths are the major contributors in determining the magnitude of the nonlinear effects. A further boost on THG is observed when we excite together more than one SLR, either at the same or at different frequencies. When such multiple resonances take place, interesting phenomena are observed, such as m…
Nonlinear metasurfaces based on coupling a locally enhanced plasmonic response to intersubband transitions of n-doped multi-quantum-wells (MQWs) have recently provided second-order susceptibilities orders of magnitude larger than any other nonlinear flat structure measured so far. Here, we present a comprehensive theory to characterize the electromagnetic response of nonlinear processes occurring in ultrathin MQW-based plasmonic metasurfaces, providing a homogeneous model that takes phase-matching at the unit-cell level and the influence of saturation and losses into account. In addition, the …
Deterministically integrating semiconductor quantum emitters with plasmonic nano-devices paves the way towards chip-scale integrable, true nanoscale quantum photonics technologies. For this purpose, stable and bright semiconductor emitters are needed, which moreover allow for CMOS-compatibility and optical activity in the telecommunication band. Here, we demonstrate strongly enhanced light-matter coupling of single near-surface ($<10\,nm$) InAs quantum dots monolithically integrated into electromagnetic hot-spots of sub-wavelength sized metal nanoantennas. The antenna strongly enhances the emi…
The heat-shielding properties of random metasurface, composed of spherical or spheroidal nanoparticles with random displacements and/or random deformation, were theoretically investigated using the finite difference time domain method. The effective coverage was defined using the total area of nanoparticles in the metasurface, and the robustness of the near-infrared light reflection against randomness was investigated. When the effective coverage was high, the near-infrared light reflection was reduced by at least 20% in both nanoparticle arrangement and shape randomness compared to the hexago…
Overcoming the diffraction limit to achieve high optical resolution is one of the main challenges in the fields of plasmonics, nanooptics and nanophotonics. In this work, we introduce novel plasmonic structures consisting of nanoantennas (nanoprisms, single bowtie nanoantennas and double bowtie nanoantennas) integrated in the center of ring diffraction gratings. Propagating surface plasmon polaritons (SPPs) are generated by the ring grating and coupled with localized surface plasmons (LSPs) at the nanoantennas exciting emitters placed in their gap. SPPs are widely used for optical waveguiding …
We study a plasmonic metasurface that supports pseudospin dependent edge states confined at a subwavelength scale, considering full electrodynamic interactions including retardation and radiative effects. The spatial symmetry of the lattice of plasmonic nanoparticles gives rise to edge states with properties reminiscent of the quantum spin Hall effect in topological insulators. However, unlike the spin-momentum locking characteristic of topological insulators, these modes are not purely unidirectional and their propagation properties can be understood by analysing the spin angular momentum of …
Using large-scale, real-time quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multi-particle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings i…
Intermixed light-matter quasiparticles - polaritons - possess unique optical properties owned to their compositional nature. These intriguing hybrid states have been extensively studied over the past decades in a wide range of realizations aiming at both basic science and emerging applications. However, recently it has been demonstrated that not only optical, but also material-related properties, such as chemical reactivity and charge transport, may be significantly altered in the strong coupling regime of light-matter interactions. Here, we show that a nanoscale system, comprised of a plasmon…
The unique gate-voltage dependent optical properties of graphene make it a promising electrically-tunable plasmonic material. In this work, we proposed in-situ control of the polarization of nanoantennas by combining plasmonic structures with an electrostatically tunable graphene monolayer. The tunable polarizer is designed based on an asymmetric cross nanoantenna comprising two orthogonal metallic dipoles sharing the same feed gap. Graphene monolayer is deposited on a Si/SiO2 substrate, and inserted beneath the nanoantenna. Our modelling demonstrates that as the chemical potential is incremen…
The breathing honeycomb lattice hosts a topologically non-trivial bulk phase due to the crystalline-symmetry of the system. Pseudospin-dependent edge states which emerge at the interface between trivial and non-trivial regions can be used for directional propagation of energy. Using the plasmonic metasurface as an example system, we probe these states in the near and far-field using a semi-analytical model. We give the conditions under which directionality is observed and show that it is source position dependent. By probing with circularly-polarized magnetic dipoles out of the plane, we first…
Laser printing with a spatial light modulator (SLM) has several advantages over conventional raster-writing and dot-matrix display (DMD) writing: multiple pixel exposure, high power endurance and existing software for computer generated holograms (CGH). We present a technique for the design and manufacturing of plasmonic metasurfaces based on ultrafast laser printing with an SLM. As a proof of principle, we have used this technique to laser print a plasmonic metalens as well as high resolution plasmonic color decorations. The high throughput holographic resonant laser printing (HRLP) approach …
We discuss the possibility of realizing utlrabroadband omnidirectional absorbers and angularly selective coherent thermal emitters based on properly patterned plasmonic metastructures. Instead of relying on resonant concentration effects that inherently limit the bandwidth, we base our design on the combination of two inherently nonresonant effects: plasmonic Brewster funneling and adiabatic plasmonic focusing. With this approach, we demonstrate compact, broadband absorption and emission spanning terahertz, infrared and optical frequencies, ideal for various energy and defense applications.
We demonstrate third harmonic generation in plasmonic antennas made of highly doped germanium and designed to be resonant in the mid infrared. Owing to the near-field enhancement, the result is an ultrafast, sub-diffraction, coherent light source tunable between 3 and 5 micrometer wavelength on a silicon substrate. To observe nonlinearity in this challenging spectral region, a high-power femtosecond laser system equipped with parametric frequency conversion in combination with an all-reflective confocal microscope setup is employed. We show spatially resolved maps of the linear scattering cros…
Acoustic vibrations at the nanoscale (GHz-THz frequencies) and their interactions with electrons, photons and other excitations are the heart of an emerging field in physics: nanophononics. The design of ultrahigh frequency acoustic-phonon transducers, with tunable frequency, and easy to integrate in complex systems is still an open and challenging problem for the development of acoustic nanoscopies and phonon lasers. Here we show how an optimized plasmonic metasurface can act as a high-frequency phonon transducer. We report pump-probe experiments in metasurfaces composed of an array of gold n…
We study plasmonic excitations in the limit of few electrons, in one-atom thick sodium chains, and characterize them based on collectivity. We also compare the excitations to classical localised plasmon modes and find for the longitudinal mode a quantum-classical transition around 10 atoms. The transverse mode appears at much higher energies than predicted classically for all chain lengths. The electric field enhancement is also considered which is made possible by considering the effects of electron-phonon coupling on the broadening of the electronic spectra. Large field enhancements are poss…
Nanoantennas for visible and infrared radiation can strongly enhance the interaction of light with nanoscale matter by their ability to efficiently link propagating and spatially localized optical fields. This ability unlocks an enormous potential for applications ranging from nanoscale optical microscopy and spectroscopy over solar energy conversion, integrated optical nanocircuitry, opto-electronics and density-ofstates engineering to ultra-sensing as well as enhancement of optical nonlinearities. Here we review the current understanding of optical antennas based on the background of both we…
Planar chiral nanoantenna for excitation-chirality-controlled hot spot modulation and emitter-coupled circularly polarized emission
Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Abbe Center of Photonics, Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学阿贝光学中心）；Leibniz Institute of Photonic Technology（莱布尼茨光子技术研究所）；University of Würzburg（维尔茨堡大学）；The Australian National University（澳大利亚国立大学）；Academia Sinica（中央研究院）；National Yang Ming Chiao Tung University（国立阳明交通大学）
Active control of light-matter interactions in semiconductors is critical for realizing next generation optoelectronic devices, with tunable control of the systems optical properties via external fields. The ability to manipulate optical interactions in active materials coupled to cavities via geometrical parameters, which are fixed along with dynamic control with applied fields opens up possibilities of controlling exciton lifetimes, oscillator strengths and their relaxation properties. Here, we demonstrate electrical control of exciton-plasmon polariton coupling strength of a two-dimensional…
A local model of the dielectric response of a metal predicts that singular surfaces, such as sharp-edged structures, have a continuous absorption spectrum and extreme concentration of energy at the singularity. Here we show that nonlocality drastically alters this picture: the spectrum is now discrete and energy concentration, though still substantial, is greatly reduced.
Geometrical singularities in plasmonic metasurfaces have recently been proposed for the enhancement of light-matter interactions, owing to their broadband light-harvesting properties and extreme plasmon confinement. However, the large plasmon momenta thus achieved lead to failure of local descriptions of the optical response of metals. Here we study a class of metasurfaces consisting of a periodic metal slab with a smooth modulation of its thickness. When the thinnest part shrinks, the two surfaces almost touch, forming a near-singular point. Using transformation optics, we show analytically h…
Optical interactions have an important impact on the optical response of nanostructures in complex environments. Accounting for interactions in large ensembles of structures requires computationally demanding numerical calculations. In particular if no periodicity can be exploited, full field simulations can become prohibitively expensive. Here we propose a method for the numerical description of aperiodic assemblies of plasmonic nanostructures. Our approach is based on dressed polarizabilities, which are conventionally very expensive to calculate, a problem which we alleviate using a deep con…
We demonstrate inverse design of plasmonic nanoantennas for directional light scattering. Our method is based on a combination of full-field electrodynamical simulations via the Green dyadic method and evolutionary optimization (EO). Without any initial bias, we find that the geometries reproducibly found by EO, work on the same principles as radio-frequency antennas. We demonstrate the versatility of our approach by designing various directional optical antennas for different scattering problems. EO based nanoantenna design has tremendous potential for a multitude of applications like nano-sc…
We suggest a hybrid plasmonic device consisting of a bimodal metallic nanoantenna coupled to an incoherently pumped quantum emitter. This hybrid device emits light into the two modes entangled in the number of photons. The process is a prime example where losses are turned from a nuisance into something beneficial, since, even though counterintuitively, the entanglement is enabled by strong incoherent processes, i.e. dominant scattering and absorption rates of the nanoantenna. Both, the high emission rate and the degree of entanglement of the emitted light are insensitive with respect to imper…
