Gradient metasurfaces: a review of fundamentals and applications.

In the wake of intense research on metamaterials the two-dimensional analogue, known as metasurfaces, has attracted progressively increasing attention in recent years due to the ease of fabrication and smaller insertion losses, while enabling an unprecedented control over spatial distributions of transmitted and reflected optical fields. Metasurfaces represent optically thin planar arrays of resonant subwavelength elements that can be arranged in a strictly or quasi periodic fashion, or even in an aperiodic manner, depending on targeted optical wavefronts to be molded with their help. This paper reviews a broad subclass of metasurfaces, viz. gradient metasurfaces, which are devised to exhibit spatially varying optical responses resulting in spatially varying amplitudes, phases and polarizations of scattered fields. Starting with introducing the concept of gradient metasurfaces, we present classification of different metasurfaces from the viewpoint of their responses, differentiating electrical-dipole, geometric, reflective and Huygens' metasurfaces. The fundamental building blocks essential for the realization of metasurfaces are then discussed in order to elucidate the underlying physics of various physical realizations of both plasmonic and purely dielectric metasurfaces. We then overview the main applications of gradient metasurfaces, including waveplates, flat lenses, spiral phase plates, broadband absorbers, color printing, holograms, polarimeters and surface wave couplers. The review is terminated with a short section on recently developed nonlinear metasurfaces, followed by the outlook presenting our view on possible future developments and perspectives for future applications.

Third-order gap plasmon based metasurfaces for visible light.

Efficient control and manipulation of light using metasurfaces requires high fabrication accuracy that becomes progressively demanding when decreasing the operation wavelength. Considering gap surface plasmon (GSP) based metasurfaces, we demonstrate that the metasurfaces, which utilize the third-order GSP resonance and thereby involve relatively large nanobricks, can successfully be used for efficient polarization-controlled steering of visible light. The reflection amplitude and phase maps for a 450 nm period array of 50 nm thick nanobricks placed atop a 40 nm thick silica layer supported by an optically thick gold film are calculated for the operation wavelength of 633 nm. Exploiting the occurrence of the third-order GSP resonance for nanobricks having their lengths close to 300 nm, we design the phase-gradient metasurface, representing an array of (450 x 2250 nm2) supercells made of 5 nanobricks with different dimensions, to operate as a polarization beam splitter for linearly polarized light. The fabricated polarization beam splitter is characterized using a supercontinuum light source at the normal light incidence and found to exhibit a polarization contrast ratio of up to 40 dB near the design wavelength of 633 nm while showing better than 20 dB contrast in the range of 550 - 650 nm for both polarizations. The diffraction efficiency experimentally measured at normal incidence exceeds 10% (20% in simulations) at the design wavelength of 633 nm, with the performance for the TE polarization (electric field perpendicular to the plane of diffraction) being significantly better (experimentally > 20% and theoretically > 40%) than for the TM polarization. This difference becomes even more pronounced for the light incidence deviating from normal. Finally, we discuss possible improvements of the performance of polarization beam splitters based on third-order GSP resonance as well as other potential applications of the suggested approach.

Enhanced nonresonant light transmission through subwavelength slits in metal.

We analytically describe light transmission through a single subwavelength slit in a thin perfect electric conductor screen for the incident polarization being perpendicular to the slit, and derive simple, yet accurate, expressions for the average electric field in the slit and the transmission efficiency. The analytic results are consistent with full-wave numerical calculations and demonstrate that slits of widths ∼100 nm in real metals may feature nonresonant (i.e., broadband) field enhancements of ∼100 and transmission efficiency of ∼10 at infrared or terahertz frequencies, with the associated metasurface-like array of slits becoming transparent to the incident light.

Analog computing using reflective plasmonic metasurfaces.

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 metasurfaces featuring realistic system parameters. Proof-of-principle experiments are reported along with the successful realization of a high-quality poor-man's integrator metasurface operating at the wavelength of 800 nm.

Unidirectional scattering by nanoparticles near substrates: generalized Kerker conditions.

Starting from a general description of light scattering by a nanoparticle in homogeneous surroundings and situated near a substrate, we outline the connection to multipole expansion of scattered light and derive conditions and limits on achievable half-space scattering asymmetry, including the possibility of unidirectional scattering along the propagation direction of the incident light (i.e., generalized Kerker conditions). As a way of realizing strongly asymmetric scattering, we perform a parametric study of the optical properties of disk-shaped gap-surface plasmon (GSP) resonators, consisting of a glass spacer sandwiched between two gold disks, with numerical calculations that corroborate the conditions derived from the multipole expansion. Finally, we present proof-of-principle experiments of asymmetric scattering by GSP-resonators on a glass substrate.

Subwavelength plasmonic color printing protected for ambient use.

We demonstrate plasmonic color printing with subwavelength resolution using circular gap-plasmon resonators (GPRs) arranged in 340 nm period arrays of square unit cells and fabricated with single-step electron-beam lithography. We develop a printing procedure resulting in correct single-pixel color reproduction, high color uniformity of colored areas, and high reproduction fidelity. Furthermore, we demonstrate that, due to inherent stability of GPRs with respect to surfactants, the fabricated color print can be protected with a transparent dielectric overlay for ambient use without destroying its coloring. Using finite-element simulations, we uncover the physical mechanisms responsible for color printing with GPR arrays and suggest the appropriate design procedure minimizing the influence of the protection layer.

Nanofocusing in circular sector-like nanoantennas.

Gold circular sector-like nanoantennas (with a radius of 500 nm and a taper angle of 60°, 90°, and 120°) on glass are investigated in a near-infrared wavelength range (900 - 2100 nm). Amplitude- and phase-resolved near-field images of circular sector-like antenna modes at telecom wavelength feature a concentric circular line of phase contrast, demonstrating resonant excitation of a standing wave of counter-propagating surface plasmons, travelling between a tip and opposite circular edge of the antenna. Transmission spectra obtained in the range 900 - 2100 nm are in good agreement with numerical simulations, revealing the main feature of this antenna configuration, viz., the resonance wavelength, in contrast to triangular antennas, does not depend on the taper angle and is determined only by the sector radius. This feature together with a robust and easily predictable frequency response makes circular sector-like nanoantennas very promising for implementing bowtie antennas and attractive for many applications.

Scaling in light scattering by sharp conical metal tips.

Using the electrostatic approximation, we analyze electromagnetic fields scattered by sharp conical metal tips, which are illuminated with light polarized along the tip axis. We establish scaling relations for the scattered field amplitude and phase, and verify the validity with numerical simulations. Analytic expressions for the wavelength at which the scattered field near the tip changes its direction and for the field decay near the tip extremity are obtained, relating these characteristics to the cone angle and metal permittivity. The results obtained have important implications for various tip-enhanced phenomena, ranging from Raman and scattering near-field imaging to photoemission spectroscopy and nano-optical trapping.

Broadband focusing flat mirrors based on plasmonic gradient metasurfaces.

We demonstrate that metal-insulator-metal configurations, with the top metal layer consisting of a periodic arrangement of differently sized nanobricks, can be designed to function as broadband focusing flat mirrors. Using 50-nm-high gold nanobricks arranged in a 240-nm-period lattice on the top of a 50-nm-thick layer of silicon dioxide deposited on a continuous 100-nm-thick gold film, we realize a 17.3 × 17.3 µm(2) flat mirror that efficiently reflects (experiment: 14-27%; theory: 50-78%) and focuses a linearly polarized (along the direction of nanobrick size variation) incident beam in the plane of its polarization with the focal length, which changes from ~15 to 11 µm when tuning the light wavelength from 750 to 950 nm, respectively. Our approach can easily be extended to realize the radiation focusing in two dimensions as well as other optical functionalities by suitably controlling the phase distribution of reflected light.

Efficient and broadband quarter-wave plates by gap-plasmon resonators.

We demonstrate numerically that metal-insulator-metal (MIM) configurations in which the top metal layer consists of a periodic arrangement of nanobricks, thus facilitating gap-surface plasmon resonances, can be designed to function as efficient and broadband quarter-wave plates in reflection by a proper choice of geometrical parameters. Using gold as the metal, we demonstrate quarter-wave plate behavior at λ ~/= 800 nm with an operation bandwidth of 160 nm, conversion efficiency of 82%, and angle of linear polarization fixed throughout the entire bandwidth. This work also includes a detailed analytical and numerical study of the optical properties and underlying physics of structured MIM configurations.

Plasmonic metasurfaces for efficient phase control in reflection.

We numerically study the optical properties of metal-insulator-metal resonators and metasurfaces, emphasizing the presence of gap-surface plasmon (GSP) resonances and their connection to the optical response. In relation to birefringent metal-backed metasurfaces, we show how a combination of metal nanobrick and nanocross elements allows one to fully control the phase of reflected light for two orthogonal polarizations simultaneously. The approach is exemplified by the design of a gradient birefringent metasurface that reflects two orthogonal polarization states into +2 and -3 diffraction order, respectively, with a reflectivity up to ~ 80% and in a broad wavelength range around the design wavelength of 800 nm. Finally, we introduce the concept of metascatterers, which are wavelength-sized polarization-sensitive scatterers.

Broadband plasmonic half-wave plates in reflection.

We demonstrate, both numerically and experimentally, that metal-insulator-metal configurations in which the top metal layer consists of a periodic arrangement of nanobricks, thus supporting gap-surface plasmon resonances, can be designed to function as reflective broadband half-wave plates. Using gold as the metal, the constructed wave plates in the near-infrared regime show scalability, bandwidth of ~20% of the design wavelength, and theoretical reflectivity above 85%, while a reflectivity of ~50% is experimentally measured.

Accurate Post-Calibration Predictions for Noninvasive Glucose Measurements in People Using Confocal Raman Spectroscopy.

In diabetes prevention and care, invasiveness of glucose measurement impedes efficient therapy and hampers the identification of people at risk. Lack of calibration stability in non-invasive technology has confined the field to short-term proof of principle. Addressing this challenge, we demonstrate the first practical use of a Raman-based and portable non-invasive glucose monitoring device used for at least 15 days following calibration. In a home-based clinical study involving 160 subjects with diabetes, the largest of its kind to our knowledge, we find that the measurement accuracy is insensitive to age, sex, and skin color. A subset of subjects with type 2 diabetes highlights promising real-life results with 99.8% of measurements within A + B zones in the consensus error grid and a mean absolute relative difference of 14.3%. By overcoming the problem of calibration stability, we remove the lingering uncertainty about the practical use of non-invasive glucose monitoring, boding a new, non-invasive era in diabetes monitoring.

Efficient absorption of visible radiation by gap plasmon resonators.

We demonstrate experimentally a periodic array of differently-sized and circularly-shaped gap plasmon resonators (GPRs) with the average absorption ~94% for unpolarized light in the entire visible wavelength range (400-750 nm). Finite-element simulations verify that the polarization insensitive broadband absorption originates from localized gap surface plasmons whose resonant excitations only weakly depend on the angle of incidence. Arrays of GPRs also exhibit enhanced local field intensities (~115) as revealed by scanning two-photon photoluminescence microscopy, that are spectrally correlated with the minima in corresponding linear reflection spectra.

Localized spoof plasmons arise while texturing closed surfaces.

We demonstrate that textured closed surfaces, i.e., particles made of perfect electric conductors (PECs), are able to support localized electromagnetic resonances with properties resembling those of localized surface plasmons (LSPs) in the optical regime. Because of their similar behavior, we name these types of resonances as spoof LSPs. As a way of example, we show the existence of spoof LSPs in periodically textured PEC cylinders and the almost perfect analogy to optical plasmonics. We also present a metamaterial approach that captures the basic ingredients of their electromagnetic response.

Continuous layer gap plasmon resonators.

We demonstrate both theoretically and experimentally that a gold nanostrip supported by a thin dielectric (silicon dioxide) film and a gold underlay forms an efficient (Fabry-Perot) resonator for gap surface plasmons. Periodic nanostrip arrays are shown to exhibit strong and narrow resonances with nearly complete absorption and quality factors of ~15-20 in the near-infrared. Two-photon luminescence microscopy measurements reveal intensity enhancement factors of ~120 in the 400-nm-period array of 85-nm-wide gold strips atop a 23-nm-thick silica film at the resonance wavelength of ~770 nm. Excellent resonant characteristics, the simplicity of tuning the resonance wavelength by adjusting the nanostrip width and/or the dielectric film thickness and the ease of fabrication with (only) one lithography step required make the considered plasmonic configuration very attractive for a wide variety of applications, ranging from surface sensing to photovoltaics.

Plasmonic metamaterial wave retarders in reflection by orthogonally oriented detuned electrical dipoles.

We demonstrate that a pair of perpendicular electrical dipolar scatterers resonating at different frequencies can be used as a metamaterial unit cell to construct a nanometer-thin retarder in reflection, designing nanocross and nanobrick plasmonic configurations to function as reflecting quarter-wave plates at ~1520 and 770 nm, respectively. The design is corroborated experimentally with a monolayer of gold nanobricks, transforming linearly polarized incident radiation into circularly polarized radiation at ~780 nm.

Detuned electrical dipoles for plasmonic sensing.

We demonstrate that a pair of electrical dipolar scatterers resonating at different frequencies, i.e., detuned electrical dipoles, can be advantageously employed for plasmonic sensing of the environment, both as an individual subwavelength-sized sensor and as a unit cell of a periodic array. It is shown that the usage of the ratio between the powers of light scattered into opposite directions (or into different diffraction orders), which peaks at the intermediate frequency, allows one to reach a sensitivity of ≈ 400 nm/RIU with record high levels of figure of merit exceeding 200. Qualitative considerations are supported with detailed simulations and proof-of-principle experiments using lithographically fabricated gold nanorods with resonances at 800 nm.

Demonstration of scattering suppression in retardation-based plasmonic nanoantennas.

Modifications in scattering strength of and local field enhancement by retardation-based plasmonic nanoantennas when being transformed from straight nanorods to split-ring resonators are investigated experimentally. Scattering properties are characterized with linear reflection and extinction spectroscopy of nanoantenna arrays, whereas local field enhancements are evaluated for individual nanoantennas using two-photon-excited photoluminescence (TPL) microscopy. The linear and nonlinear optical characterizations reveal that the optical response of nanoantennas is determined by the interference of counter-propagating short-range surface plasmon polaritons (SR-SPP) and that the transformation of nanorods into split-rings by bending significantly influences the scattering strength. Importantly, strong suppression of scattering for the fundamental SR-SPP resonance is observed when the bend radius is decreased, a feature that is attributed to the decrease in the nanoantenna electric-dipole response when bending the nanorods. The experimental observations are corroborated with numerical simulations using the finite-element method.

Critical-depth Raman spectroscopy enables home-use non-invasive glucose monitoring.

One of the most ambitious endeavors in the field of diabetes technology is non-invasive glucose sensing. In the past decades, a number of different technologies have been assessed, but none of these have found its entry into general clinical use. We report on the development of a table-top confocal Raman spectrometer that was used in the home of patients with diabetes and operated for extended periods of time unsupervised and without recalibration. The system is based on measurement of glucose levels at a 'critical depth' in the skin, specifically in the interstitial fluid located below the stratum corneum but above the underlying adipose tissue layer. The region chosen for routine glucose measurements was the base of the thumb (the thenar). In a small clinical study, 35 patients with diabetes analyzed their interstitial fluid glucose for a period of 60 days using the new critical-depth Raman (CD-Raman) method and levels were correlated to reference capillary blood glucose values using a standard finger-stick and test strip product. The calibration of the CD-Raman system was stable for > 10 days. Measurement performance for glucose levels present at, or below, a depth of ~250µm below the skin surface was comparable to that reported for currently available invasive continuous glucose monitors. In summary, using the CD-Raman technology we have demonstrated the first successful use of a non-invasive glucose monitor in the home.