Hyperpolarizability of plasmonic meta-atoms in metasurfaces
M. Saad Bin-Alam, Joshua Baxter, Kashif M. Awan, Antti Kiviniemi, Yaryna Mamchur, Antonio Calà Lesina, Kosmas L. Tsakmakidis, Mikko J. Huttunen, Lora Ramunno, Ksenia Dolgaleva
Plasmonic metasurfaces are promising as enablers of nanoscale nonlinear optics and flat nonlinear optical components. Nonlinear optical responses of such metasurfaces are determined by the nonlinear optical properties of individual nanostructured plasmonic meta-atoms, which are the building blocks of the metasurfaces. Unfortunately, no simple methods exist to determine the nonlinear coefficients (hyperpolarizabilities) of the meta-atoms hindering designing of nonlinear metasurfaces. Here, we develop the equivalent RLC circuit model of such meta-atoms to estimate their second-order nonlinear optical parameter i.e. the first-order hyperpolarizability in the optical spectral range. In parallel, we extract from second-harmonic generation experiments the spectrum of the 1st-order hyperpolarizabilities of individual meta-atoms consisting of asymmetrically shaped (elongated) plasmonic nanoprisms. Moreover, we verify our results using nonlinear hydrodynamic-FDTD and with calculations based on nonlinear scattering theory. All three approaches: analytical, experimental, and computational, yield results that agree very well. Our empirical RLC model can thus be used as a simple tool to enable efficient design of nonlinear plasmonic metasurfaces.
Metasurfaces, and in particular those containing plasmonic-based metallic elements, constitute a particularly attractive set of materials. By means of modern nanolithographic fabrication techniques, flat, ultrathin optical elements may be constructed. However, in spite of their strong optical nonlinearities, plasmonic metasurfaces have so far been investigated mostly in the linear regime. Here we introduce full nonlinear phase control over plasmonic elements in metasurfaces. We show that for nonlinear interactions in a phase-gradient nonlinear metasurface a new anomalous nonlinear phase matchi…
A hybrid plasmonic-dielectric metasurface is proposed in order to manipulate beam propagation in desired manners. The metasurface is composed of patterned hybrid graphene-silicon nano-disks deposited on a low-index substrate, namely silica. It is shown that the proposed hybrid metasurface simultaneously benefits from the advantages of graphene-based metasurfaces and dielectric ones. Specially, we show that the proposed hybrid metasurface not only provides reconfigurability, just like previously proposed graphene-based metasurfaces, but also similar to dielectric metasurfaces it is low loss and…
Multiresonant metasurfaces could enable many applications in filtering, sensing and nonlinear optics. However, developing a metasurface with more than one high-quality-factor or high-Q resonance at designated resonant wavelengths is challenging. Here, we experimentally demonstrate a plasmonic metasurface exhibiting different, narrow surface lattice resonances by exploiting the polarization degree of freedom where different lattice modes propagate along different dimensions of the lattice. The surface consists of aluminum nanostructures in a rectangular periodic lattice. The resulting surface l…
Parity-Time (PT) symmetric optical structures exhibit several unique and interesting characteristics with the most popular being exceptional points. While the emerging concept of PT-symmetry has been extensively investigated in bulky photonic designs, its exotic functionalities in nanophotonic non-Hermitian plasmonic systems still remain relatively unexplored. Towards this goal, in this work we analyze the unusual properties of a plasmonic Huygens metasurface composed of an array of active metal-dielectric core-shell nanoparticles. By calculating the reflection and transmission coefficients of…
Motivated by the recent renewed interest in compact analog computing using light and metasurfaces (Silva, A. et al., Science 2014, 343, 160-163), we suggest a practical approach to its realization that involves reflective metasurfaces consisting of arrayed gold nanobricks atop a subwavelength-thin dielectric spacer and optically-thick gold film, a configuration that supports gap-surface plasmon resonances. Using well established numerical routines, we demonstrate that these metasurfaces enable independent control of the light phase and amplitude, and design differentiator and integrator metasu…
Plasmonic nanostructures hold promise for the realization of ultra-thin sub-wavelength devices, reducing power operating thresholds and enabling nonlinear optical functionality in metasurfaces. However, this promise is substantially undercut by absorption introduced by resistive losses, causing the metasurface community to turn away from plasmonics in favour of alternative material platforms (e.g., dielectrics) that provide weaker field enhancement, but more tolerable losses. Here, we report a plasmonic metasurface with a quality-factor (Q-factor) of 2340 in the telecommunication C band by exp…
A switchable metasurface composed of plasmonic split ring resonators and a dye-doped liquid crystal is developed. The transmission of the metasurface in the infrared spectral range can be changed by illuminating the dye-doped liquid crystal with light in the visible spectral range. The effect is particularly efficient in the case of hybrid alignment of the liquid crystal, i. e. alignment of the director perpendicular to the surface on one substrate and parallel alignment on the counter substrate. This all-optical switching effect can be attributed to the behavior described in earlier works as …
Herein, we investigate the optical properties of quantum plasmonic metasurfaces composed of metallic nano-objects with subnanometer gaps according to the time-dependent density functional theory, a fully quantum mechanical approach. When the quantum and classical descriptions are compared, the transmission, reflection, and absorption rates of the metasurface exhibit substantial differences at shorter gap distances. The differences are caused by electron transport through the gaps of the nano-objects. The electron transport has profound influences for gap distances less-than or approximately 0.…
We report here and experimentally demonstrate an actively controlled gatetunable plasmonic metasurface operating in the visible region of the electromagnetic spectrum, where strikingly the operating voltages for reflectance modulation are much less than 1V. The electrically tunable metasurface consists of inverse dolmen structures (iDolmen) patterned on silver and chromium on a quartz substrate and subsequently covered with a 5 nm thin layer of Al2O3 followed by a 110 nm indium tin oxide (ITO) layer, which acts as a transparent electrode. Our designed structures show up to 78 percent change in…
Plasmonic metasurfaces enable simultaneous control of the phase, momentum, amplitude and polarisation of light and hence promise great utility in realisation of compact photonic devices. In this paper, we demonstrate a novel chip-scale device suitable for simultaneous polarisation and spectral measurements through use of six integrated plasmonic metasurfaces (IPMs), which diffract light with a given polarisation state and spectral component into well-defined spatial domains. Full calibration and characterisation of our device is presented, whereby good spectral resolution and polarisation accu…
Resonant metasurfaces are devices composed of nanostructured sub-wavelength scatterers that generate narrow optical resonances, enabling applications in filtering, nonlinear optics, and molecular fingerprinting. It is highly desirable for these applications to incorporate such devices with multiple, high-quality-factor resonances; however, it can be challenging to obtain more than a pair of narrow resonances in a single plasmonic surface. Here, we demonstrate a multi-resonant metasurface that operates by extending the functionality of surface lattice resonances, which are the collective respon…
On-chip spectral imaging based on engineered spectral modulation and computational spectral reconstruction provides a promising scheme for portable spectral cameras. However, the angle dependence of modulation units results in the angle sensitivity of spectral imaging, which limits its practical applications. Here, we proposed a design for angle-robust spectral recovery based on a group of topology-optimized plasmonic metasurface units under a 30° field-of-view, and demonstrate angle-insensitive on-chip spectral imaging in the wavelength range of 450 to 750 nm for average polarization. Further…
A new configuration for metasurface construction is presented to achieve multi-functional capabilities including perfect absorption, bio/chem sensing, and surface-mode lasing. The reciprocal plasmonic metasurfaces discussed here are composed of two plasmonic surfaces of reciprocal geometries separated by a dielectric spacer. Compared to conventional metasurfaces this simple geometry exhibits an enhanced optical performance. The discussed reciprocal metasurface design further enables effective structural optimization and allows for a simple and scalable fabrication. The physical principle and p…
Plasmonic metasurfaces are investigated that consist of a sub wavelength line pattern in an ultrathin (~ 10 nm) silver film, designed for extraordinarily suppressed transmission (EOST) in the visible spectral range. Measurements with a near-field scanning optical microscope (NSOM) demonstrate that far field irradiation creates resonant excitations of antenna like (bright) modes that are localized on the metal ridges. In contrast, bound (dark) surface plasmon polaritons (SPPs) launched from an NSOM tip propagate well across the metasurface, preferentially perpendicular to the grating lines.
The concept of optical phase discontinuities is applied to the design and demonstration of aberration-free planar lenses and axicons, comprising a phased array of ultrathin subwavelength spaced optical antennas. The lenses and axicons consist of radial distributions of V-shaped nanoantennas that generate respectively spherical wavefronts and non-diffracting Bessel beams at telecom wavelengths. Simulations are also presented to show that our aberration-free designs are applicable to high numerical aperture lenses such as flat microscope objectives.
Chiral nanophotonic devices are promising candidates for chiral molecules sensing, polarization diverse nanophotonics and display technologies. Active chiral nanophotonic devices, where the optical chirality can be controlled by an external stimulus has triggered great research interest. However, efficient modulation of the optical chirality has been challenging. Here, we demonstrate switching of the extrinsic chirality by applied magnetic fields in a magneto-plasmonic metasurface device based on a magneto-optical oxide material, Ce1Y2Fe5O12 (Ce:YIG). Thanks to the low optical loss and strong …
Plasmonic metasurfaces provide an effective way to increase the efficiency of several nonlinear processes while maintaining nanoscale dimensions. In this work, nonlinear metasurfaces based on film-coupled silver nanostripes loaded with Kerr nonlinear material are proposed to achieve efficient four-wave mixing (FWM). Highly localized plasmon resonances are formed in the nanogap between the metallic film and nanostripes. The local electric field is dramatically enhanced in this subwavelength nanoregion. These properties combined with the relaxed phase matching condition due to the ultrathin area…
Classical emulation of a ubiquitous quantum mechanical phenomenon of double-continuum Fano (DCF) interference using metasurfaces is experimentally realized by engineering the near-field interaction between two bright and one dark plasmonic modes. The competition between the bright modes, with one of them effectively suppressing the Fano interference for the orthogonal light polarization, is discovered and explained by the analytic theory of the plasmonic DCF interference, which is further applied to predicting the circularly dichroic optical field concentration by plasmonic metasurfaces.
Plasmonic resonances in metallic nanostructures have been shown to drastically enhance local electromagnetic fields, and thereby increase the efficiency of nonlinear optical phenomena, such as second harmonic generation (SHG). While it has been experimentally observed that enhanced fields can significantly boost SHG, to date it proved difficult to probe electrical and magnetic resonances in one and the same nanostructure. This however is necessary to directly compare relative contributions of electrical and magnetic components of SHG enhancement. In this paper we report an experimental study o…
Nonreciprocity is important for optical information processing, full-duplex communications, and protection of sensitive laser equipment from unwanted reflections. However, it is very challenging to obtain strong nonreciprocal response in optical frequencies, especially when nanoscale configurations are considered. In this work, we solve this problem by demonstrating a compact bifacial plasmonic metasurface that acts as a new ultrathin nonreciprocal transmission filter at near-infrared frequencies. The proposed nanostructure is simple to be practically implemented, since it is composed of two s…
Fully reconfigurable metasurfaces would enable new classes of optical devices that provide unprecedented control of electromagnetic beamforms. The principal challenge for achieving reconfigurability is the need to generate large tunability of subwavelength, low-Q metasurface resonators. Here, we demonstrate large refractive index tuning can be efficiently facilitated at mid-infrared wavelengths using novel temperature-dependent control over free-carrier refraction. In doped InSb we demonstrate nearly two-fold increase in the electron effective mass leading to a positive refractive index shift …
Nonlinear metasurface holography shows the great potential of metasurfaces to control the phase, amplitude, and polarization of light while simultaneously converting the frequency of the light. The possibility of tailoring the scattering properties of a coherent beam, as well as the scattering properties of nonlinear signals originating from the meta-atoms facilitates a huge degree of freedom in beam shaping application. Recently, several approaches showed that virtual objects or any kind of optical information can be generated at a wavelength different from the laser input beam. Here, we demo…
Bidirectional nanoantennas are of key relevance for advanced functionalities to be implemented at the nanoscale, and in particular for color routing in an ultracompact flat-optics configuration. Here we demonstrate a novel approach avoiding complex collective geometries and/or restrictive morphological parameters, based on cross-polarized detuned plasmonic nanoantennas in a uniaxial (quasi-1D) bimetallic configuration. The nanofabrication of such a flat-optics system is controlled over a large-area (cm^2) by a novel self-organized technique exploiting ion-induced nanoscale wrinkling instabilit…
Fano resonances are features in transmissivity/reflectivity/absorption that owe their origin to the interaction between a bright resonance and a dark (i.e., sub-radiant) narrower resonance, and may emerge in the optical properties of planar two-dimensional (2D) periodic arrays (metasurfaces) of plasmonic nanoparticles. In this Letter, we provide a thorough assessment of their nature for the general case of normal and oblique plane wave incidence, highlighting when a Fano resonance is affected by the mutual coupling in an array and its capability to support free modal solutions. We analyze the …
The spin-dependent routing of surface plasmons on metal by use of mirror symmetric periodic metasurface is presented and analyzed. We incorporate the intrinsic transverse spin angular momentum of the plasmonic wave in order to efficiently couple the incident light carrying circular polarization to a desired direction. The combination of the oblique incidence of polarized light with the accurately designed momentum matching properties of the grating provides a perfect way to achieve a spin-locking metasurface that routes the plasmonic beams.
The nonlinear optical response of materials to exciting light is enhanced by resonances between the incident laser frequencies and the energy levels of the excited material. Traditionally, in molecular nonlinear spectroscopy one tunes the input laser frequencies to the molecular energy levels for highly enhanced doubly or triply resonant interactions. With metasurfaces the situation is different, and by proper design of the nanostructures, one may tune the material energy levels to match the incoming laser frequencies. Here we use multi-parameter genetic algorithm methodologies to optimize the…
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…
Measuring light's state of polarization is an inherently difficult problem, since the phase information between orthogonal polarization states is typically lost in the detection process. In this work, we bring to the fore the equivalence between normalized Stokes parameters and diffraction contrasts in appropriately designed phase-gradient birefringent metasurfaces and introduce a concept of all-polarization birefringent metagratings. The metagrating, which consists of three interweaved metasurfaces, allows one to easily analyze an arbitrary state of light polarization by conducting simultaneo…
Topologically protected plasmonic modes located inside topological bandgaps are attracting increasing attention, chiefly due to their robustness against disorder-induced backscattering. Here, we introduce a bilayer graphene metasurface that possesses plasmonic topological valley interface modes when the mirror symmetry of the metasurface is broken by horizontally shifting the lattice of holes of the top layer of the two freestanding graphene layers in opposite directions. In this configuration, light propagation along the domain-wall interface of the bilayer graphene metasurface shows unidirec…
Resonances in optical systems are useful for many applications, such as frequency comb generation, optical filtering, and biosensing. However, many of these applications are difficult to implement in optical metasurfaces because traditional approaches for designing multi-resonant nanostructures require significant computational and fabrication efforts. To address this challenge, we introduce the concept of Fourier lattice resonances (FLRs) in which multiple desired resonances can be chosen a priori and used to dictate the metasurface design. Because each resonance is supported by a distinct su…
Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically pr…
Recent investigations on optical nonlinearities of plasmonic materials suggest their responses may be even beyond the usual perturbative description. To better understand these surprisingly strong responses, we develop here a simple but general approach to describe the nonlinear optical response of plasmonic materials up to $n$th perturbation order. We apply the approach to understand spectral broadening occurring in resonant metasurfaces and investigate the enhancement of high-harmonic generation from multiply-resonant metasurfaces, predicting an over million-fold enhancement of higher harmon…
Plasmonic metasurfaces represent a promising platform for enhancing light-matter interaction. Active control of the optical response of metasurfaces is desirable for applications such as beam-steering, modulators and switches, biochemical sensors, and compact optoelectronic devices. Here we use a plasmonic metasurface with two Fano resonances to enhance the interaction of infrared light with electrically controllable single layer graphene. It is experimentally shown that the narrow spectral width of these resonances, combined with strong light/graphene coupling, enables reflectivity modulation…
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…
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 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 …
Recently, nonlinear hybrid metasurface comes into an attractive new concept in the research of nanophotonics and nanotechnology. It is composed of semiconductors with an intrinsically large nonlinear susceptibility and traditional plasmonic metasurfaces, offering opportunities for efficiently generating and manipulating nonlinear optical responses. A high second-harmonic generation (SHG) conversion efficiency has been demonstrated in the mid-infrared region by using multi-quantum-well (MQW) based plasmonic metasurfaces. However, it has yet to be demonstrated in the visible region. Here we pres…
We realize and investigate a nonlinear metasurface taking advantage of intersubband transitions in ultranarrow GaN/AlN multi-quantum well heterostructures. Owing to huge band offsets, the structures offer resonant transitions in the telecom window around 1.55 $μ$m. These heterostructures are functionalized with an array of plasmonic antennas featuring cross-polarized resonances at these near-infrared wavelengths and their second harmonic. This kind of nonlinear metasurface allows for substantial second-harmonic generation at normal incidence which is completely absent for an antenna array with…
The nonlinear processes of frequency conversion like second harmonic generation (SHG) usually obey certain selection rules, resulting from the preservation of different kind of physical quantities, e.g., the angular momentum. For SHG created by monolayer of transition-metal dichalcogenides (TMDCs) like WS2, the valley-exciton locked selection rule predicts an SHG signal in the cross-polarization state. By combining plasmonic nanostructures with a monolayer of TMDC, a hybrid metasurface is realized which affects this nonlinear process due to an additional polarization conversion process. Here, …
Nonlinear metasurfaces offer new paradigm for boosting optical effect beyond limitations of conventional materials. In this work, we present an alternative way to produce pronounced third-harmonic generation (THG) based on nonlinear field resonances rather than linear field enhancement, which is a typical strategy for achieving strong nonlinear response. By designing and studying a nonlinear plasmonic-graphene metasurface at terahertz regime with hybrid guided modes and bound states in the continuum modes, it is found that a THG with a narrow bandwidth can be observed, thanks to the strong res…
High-quality flat optical elements require efficient light deflection to large angles and over a wide wavelength spectrum. Although phase gradient metasurfaces achieve this by continuously adding phase shifts in the range of 0 to 2π to the electric field with subwavelength-sized scatterers, their performance is limited by the spatial resolution of phase modulation at the interface. Here, we introduce a new class of metasurfaces based on a general formulation, where the phase shifts cover less than the full 0-2π range, offering significant advantages. More specifically, this approach allows the…
The index of refraction governs the flow of light through materials. At visible and near infrared wavelengths the real part of the refractive index is limited to less than 3 for naturally occurring transparent materials, fundamentally restricting applications. Here, we carried out experiments to study the upper limit of the effective refractive index of self-assembled metasurfaces at visible and near-infrared wavelengths. The centimeter-scale metasurfaces were made of a hexagonally close packed (hcp) monolayer of gold nanospheres coated with tunable alkanethiol ligand shells, controlling the i…
