Adiabatic Nanofocusing Research Articles

Fabrication of pyramid-shaped gold tip for adiabatic nanofocusing of surface plasmon polaritons

Scattering-type scanning near-field optical microscopy based on adiabatic nanofocusing of surface plasmon polaritons (SPPs) is a powerful technique that can achieve free-background nanoscale optical resolution of material. However, the performance of the propagated confined modes strongly depends on the characteristic structure of the probe. Although the metallic pyramid structure provides excellent tightly confined modes, however, it is challenging to realize the required pyramid geometry. Here, we propose a simple method for fabricating a reproducible and controllable gold pyramid-shaped tip. The produced pyramid-shaped tips were made by electrochemical etching and by applying a pulse wave to the system. From a systematic study, we found that the key factor of fabrication of desired tip geometry is based on the platinum (Pt) wire shapes. Traditional circular-shaped platinum ring electrodes are used for gold tip fabrication in an electrochemical etching. In our method, we bent the Pt wire into a triangular shape as the electrode for the etching process. The influence of the geometrical ring shapes on the fabrication of the Au tip structure is investigated. The gold tip structure was optimized by controlling the Pt ring shape, and the desired pyramid-shaped gold tip was achieved with a yield of 70%. The obtained etched pyramid-shaped tips were then mounted along the side of one of the arms of a quartz tuning fork force sensor to test their performance for shear-force topographical image and for guiding SPPs along the pyramid wedge based on adiabatic nanofocusing microscopy. The result shows topographical images of indium tin oxide with a spatial resolution smaller than 20 nm. Furthermore, we experimentally demonstrate the generation of the SPPs that propagated adiabatically along the wedge of an appropriate fabricated pyramid-shaped tip toward a nanometer-size spot at the tip apex. The demonstration of this method strongly suggests that the obtained pyramid-shaped tip will enable new experiments probing the dynamics of optical excitations of individual metallic, semiconducting, and magnetic nanostructures.

Absorption properties and mechanisms of metallic moth-eye structures

The antireflection and absorption properties of non-metallic moth-eye structures have been intensively studied, however the research on those of metallic moth-eye structures, especially their absorption mechanisms, is far from enough. In this paper, the absorption properties and mechanisms of a metallic Au moth-eye structure are studied in detail. The results show that broadband perfect absorption covering the entire visible to the near infrared range with polarization independence and in a wide incident angle range can be easily realized using a single-layer single-material Au moth-eye structure. As for the absorption mechanism, in the short wavelength range of 300 nm–550 nm, due to the high loss of the Au material, the antireflection effect plays a main role. While in the long wavelength range of 550 nm–1000 nm, the widely accepted absorption mechanisms (the antireflection effect as well as the cascaded multiple plasmonic resonances, and even the combination of them) cannot completely account for the broadband perfect absorption. We found that the adiabatic nanofocusing effect of the plasmonic resonances enabled by the ultra-sharp air grooves plays a key role in the absorption. It is the nanofocusing effect that effectively increases the absorption to nearly 100% in a broad wavelength band. These findings provide a deeper insight into the absorption mechanisms of metallic moth-eye structures and offer an effective guide to explore demanded excellent absorption performance.

Fourier optics with linearly tapered waveguides: Light trapping and focusing

An optical pulse asymptotically reaching zero group velocity in tapered waveguides can ultimately stop at a certain position in the taper accompanied by a strong spatial compression. This phenomenon can also be observed in spatiotemporal systems where the pulse velocity asymptotically reaches the velocity of a tapered front. The first system is well known from tapered plasmonic waveguides where adiabatic nano-focusing of light is observed. Its counterpart in the spatiotemporal system is the optical push broom effect where a nonlinear front collects and compresses the signal. Here, we use the slowly varying envelope approximation to describe such systems. We demonstrate an analytical solution for the linear taper and the piecewise linear dispersion and show that the solution in this case resembles that of an optical lens in paraxial approximation. In particular, the spatial distribution of the focused light represents the Fourier transform of the signal at the input.

Broadband Meta‐Absorber with Au/Ni Core–Shell Nanowires for Solar Vapor Generator

AbstractSolar energy has the advantages of being eco‐friendly, practically infinite, and nonreliant on chemical fuels. A solar vapor generator uses sunlight to transform a liquid stream into a vapor stream to operate a turbine for generating electricity. For efficient vapor generation, it should absorb the sunlight in broad spectrum with high absorption, and also have high photothermal conversion efficiency. In this work, Ni nanowires and Au/Ni core–shell nanowire absorbers which meet the relevant conditions are fabricated using a cost‐effective process for efficient solar vapor generation. The light is scattered and trapped in the nanowires and the electrical field is enhanced between the nanowires by the surface plasmonic gap resonance, resulting in high absorption. Also, the adiabatic nanofocusing structure generates heat at hot spots, resulting in efficient photothermal conversion. As a result, the Ni and Au/Ni core–shell nanowire absorbers respectively, absorb over 98% and 91% of the incident light in the solar spectrum. Further, the efficiency of photothermal conversion of the Au–Ni absorber under 1 Sun is found to be ≈33%. These absorbers have the potential to be applied to diverse fields, such as desalination, solar thermophotovoltaics, and metamaterials.

Plasmonic analogue of geometric diodes realizing asymmetric optical transmission.

Geometric diodes represent a relatively new class of diodes used in rectennas that rely on the asymmetry of a conducting thin film. Here, we numerically investigate a plasmonic analogue of geometric diodes to realize nanoscale optical asymmetric transmission. The device operates based on spatial symmetry breaking that relies on a unique property of surface plasmon polaritons (SPPs), namely, adiabatic nanofocusing. We show that the structure can realize on-chip asymmetric electromagnetic transmission with a total dimension of ∼2µm×6µm. We demonstrate a signal contrast of 0.7 and an asymmetric optical transmission ratio of 4.77 dB. We investigate the origin of the asymmetric transmission and show that it is due mainly to asymmetric out-coupling of SPPs to far-field photons. We highlight the role of evanescent field coupling of SPPs in undermining the asymmetric transmission efficiency and show that by adjusting the plasmonic waveguide dimensions, a signal contrast of 0.94 and an asymmetric optical transmission ratio of 5.18 dB can be obtained. Our work presents a new paradigm for on-chip nanoscale asymmetric optical transmission utilizing the unique properties of SPPs.

Double-sided and omnidirectional absorption of visible light in tapered dielectric nanostructure coated with non-noble metal.

The common complex architecture constitutes the major bottleneck of optical absorber operating on broadband spectrum. Here we demonstrate a super absorber consisting of tapered dielectric nanostructure coated with a thin-layer of non-noble metal chromium on flexible poly(ethylene terephthalate) substrate. The proposed device yields double-sided, omnidirectional, and polarization-independent absorption over the entire visible spectrum with an average efficiency more than 90% at normal incidence, and 80% at a tilt incident angle of 60°. It can be easily realized by nanoimprinting lithography combined with physical vapor deposition technique. Theoretical analysis demonstrates that the superior optical performance is ascribed to the non-resonant light absorption by using the metal-covered, closed-packed tapered nanostructure via adiabatic nanofocusing of the metal-dielectric-metal (MDM) guided modes excited by scattering of the gradually changing nanostructure. For the cost-effective fabrication and material strategy, the super absorber has potential applications in a wide range of passive and active photonic devices, including inkless printing, harvesting solar energy, as well as thermal emitter and optical detector.

Ultrafast coherent nonlinear nanooptics and nanoimaging of graphene.

With its linear energy dispersion and large transition dipole matrix element, graphene is an attractive material for nonlinear optoelectronic applications. However, the mechanistic origin of its strong nonlinear response, the ultrafast coherent dynamics and the associated nanoscale phenomena have remained elusive due to a lack of suitable experimental techniques. Here, using adiabatic nanofocusing and imaging, we study the broadband four-wave mixing (FWM) response of graphene with nanometre and femtosecond spatio-temporal resolution. We detect a nonlinear signal enhancement at the edges and dependence on the number of layers from excitation areas as small as 104 carbon atoms. Femtosecond FWM nanoimaging and concomitant frequency-domain measurements reveal dephasing on T2 ≈ 6 ± 1 fs timescales, which we attribute to a strong electron-electron interaction. We also identify an unusual non-local FWM response on ~100-400 nm length scales, which we assign to a Doppler effect controlling the nonlinear interaction between the tip near-field momenta and the graphene electrons with high Fermi velocity. These results illustrate the distinct nonlinear nanooptical properties of graphene, expected also in related classes of two-dimensional materials, that could form the basis for improved nonlinear and ultrafast nanophotonic devices.

Enhanced Third-Order Optical Nonlinearity Driven by Surface-Plasmon Field Gradients.

Efficient nonlinear optical frequency mixing in small volumes is key for future on-chip photonic devices. However, the generally low conversion efficiency severely limits miniaturization to nanoscale dimensions. Here we demonstrate that gradient-field effects can provide for an efficient, conventionally dipole-forbidden nonlinear response. We show that a longitudinal nonlinear source current can dominate the third-order optical nonlinearity of the free electron response in gold in the technologically important near-IR frequency range where the nonlinearities due to other mechanisms are particularly small. Using adiabatic nanofocusing to spatially confine the excitation fields, from measurements of the 2ω_{1}-ω_{2} four-wave mixing response as a function of detuning ω_{1}-ω_{2}, we find up to 10^{-5} conversion efficiency with a gradient-field contribution to χ_{Au}^{(3)} of up to 10^{-19} m^{2}/V^{2}. The results are in good agreement with the theory based on plasma hydrodynamics and underlying electron dynamics. The associated increase in the nonlinear conversion efficiency with a decreasing sample size, which can even overcompensate the volume decrease, offers a new approach for enhanced nonlinear nano-optics. This will enable more efficient nonlinear optical devices and the extension of coherent multidimensional spectroscopies to the nanoscale.

Near-field coupling of gold plasmonic antennas for sub-100 nm magneto-thermal microscopy

The development of spintronic technology with increasingly dense, high-speed, and complex devices will be accelerated by accessible microscopy techniques capable of probing magnetic phenomena on picosecond time scales and at deeply sub-micron length scales. A recently developed time-resolved magneto-thermal microscope provides a path towards this goal if it is augmented with a picosecond, nanoscale heat source. We theoretically study adiabatic nanofocusing and near-field heat induction using conical gold plasmonic antennas to generate sub-100 nm thermal gradients for time-resolved magneto-thermal imaging. Finite element calculations of antenna-sample interactions reveal focused electromagnetic loss profiles that are either peaked directly under the antenna or are annular, depending on the sample’s conductivity, the antenna’s apex radius, and the tip-sample separation. We find that the thermal gradient is confined to 40 nm to 60 nm full width at half maximum for realistic ranges of sample conductivity and apex radius. To mitigate this variation, which is undesirable for microscopy, we investigate the use of a platinum capping layer on top of the sample as a thermal transduction layer to produce heat uniformly across different sample materials. After determining the optimal capping layer thickness, we simulate the evolution of the thermal gradient in the underlying sample layer and find that the temporal width is below 10 ps. These results lay a theoretical foundation for nanoscale, time-resolved magneto-thermal imaging.

Size-Reduction Template Stripping of Smooth Curved Metallic Tips for Adiabatic Nanofocusing of Surface Plasmons.

We present a new technique to engineer metallic interfaces to produce sharp tips with smooth curved surfaces and variable tip angles, as well as ridges with arbitrary contour shapes, all of which can be integrated with grating couplers for applications in plasmonics and nanophotonics. We combine template stripping, a nanofabrication scheme, with atomic layer deposition (ALD) to produce the ultrasharp nanoscale tips and wedges using only conventional photolithography. Conformal ALD coating of insulators over silicon trench molds of various shapes reduces their widths to make nanoscale features without high-resolution lithography. Along with a metal deposition and template stripping, this size-reduction scheme can mass-produce narrow and ultrasharp (<10 nm radius of curvature) metallic wedges and tips over an entire 4 in. wafer. This size-reduction scheme can create metallic tips out of arbitrary trench patterns that have smooth curved surfaces to facilitate efficient adiabatic nanofocusing which will benefit applications in near-field optical spectroscopy, plasmonic waveguides, particle trapping, hot-electron plasmonics, and nonlinear optics.

Omnidirectional optical attractor in structured gap-surface plasmon waveguide.

An optical attractor based on a simple and easy to fabricate structured metal-dielectric-metal (SMDM) waveguide is proposed. The structured waveguide has a variable thickness in the vicinity of an embedded microsphere and allow for adiabatic nano-focusing of gap-surface plasmon polaritons (GSPPs). We show that the proposed system acts as an omnidirectional absorber across a broad spectral range. The geometrical optics approximation is used to provide a description of the ray trajectories in the system and identify the singularity of the deflection angle at the photon sphere. The analytical theory is validated by full-wave numerical simulations demonstrating adiabatic, deep sub-wavelength focusing of GSPPs and high local field enhancement. The proposed structured waveguide is an ideal candidate for the demonstration of reflection free omnidirectional absorption of GSPP in the optical and infrared frequency ranges.

Adiabatic Nanofocusing in Hybrid Gap Plasmon Waveguides on the Silicon-on-Insulator Platform.

We present an experimental demonstration of a new class of hybrid gap plasmon waveguides on the silicon-on-insulator (SOI) platform. Created by the hybridization of the plasmonic mode of a gap in a thin metal sheet and the transverse-electric (TE) photonic mode of an SOI slab, this waveguide is designed for efficient adiabatic nanofocusing simply by varying the gap width. For gap widths greater than 100 nm, the mode is primarily photonic in character and propagation lengths can be many tens of micrometers. For gap widths below 100 nm, the mode becomes plasmonic in character with field confinement predominantly within the gap region and with propagation lengths of a few microns. We estimate the electric field intensity enhancement in hybrid gap plasmon waveguide tapers at 1550 nm by three-photon absorption of selectively deposited CdSe/ZnS quantum dots within the gap. Here, we show electric field intensity enhancements of up to 167 ± 26 for a 24 nm gap, proving the viability of low loss adiabatic nanofocusing on a commercially relevant photonics platform.

Flexible thin-film black gold membranes with ultrabroadband plasmonic nanofocusing for efficient solar vapour generation.

Solar steam generation has been achieved by surface plasmon heating with metallic nanoshells or nanoparticles, which have inherently narrow absorption bandwidth. For efficient light-to-heat conversion from a wider solar spectrum, we employ adiabatic plasmonic nanofocusing to attain both polarization-independent ultrabroadband light absorption and high plasmon dissipation loss. Here we demonstrate large area, flexible thin-film black gold membranes, which have multiscale structures of varying metallic nanoscale gaps (0–200 nm) as well as microscale funnel structures. The adiabatic nanofocusing of self-aggregated metallic nanowire bundle arrays produces average absorption of 91% at 400–2,500 nm and the microscale funnel structures lead to average reflection of 7% at 2.5–17 μm. This membrane allows heat localization within the few micrometre-thick layer and continuous water provision through micropores. We efficiently generate water vapour with solar thermal conversion efficiency up to 57% at 20 kW m−2. This new structure has a variety of applications in solar energy harvesting, thermoplasmonics and related technologies.

Ultrafast Electron Emission from a Sharp Metal Nanotaper Driven by Adiabatic Nanofocusing of Surface Plasmons.

We report photoelectron emission from the apex of a sharp gold nanotaper illuminated via grating coupling at a distance of 50 μm from the emission site with few-cycle near-infrared laser pulses. We find a fifty-fold increase in electron yield over that for direct apex illumination. Spatial localization of the electron emission to a nanometer-sized region is demonstrated by point-projection microscopic imaging of a silver nanowire. Our results reveal negligible plasmon-induced electron emission from the taper shaft and thus efficient nanofocusing of few-cycle plasmon wavepackets. This novel, remotely driven emission scheme offers a particularly compact source of ultrashort electron pulses of immediate interest for miniaturized electron microscopy and diffraction schemes with ultrahigh time resolution.

Adiabatic nanofocusing of the fundamental modes in plasmonic parabolic potentials

We investigate the adiabatic nanofocusing of the fundamental modes in plasmonic parabolic potentials. The potentials are obtained in the metal–dielectric–metal structure, of which the dielectric layer width is modulated quadratically in the horizontal direction and linearly in the longitudinal direction. In such a structure, light is compressed in both transverse directions due to increasingly stronger parabolic potentials and decreasing dielectric layer width. We show by both closed form analytical descriptions and numerical simulations that there is a critical tapering angle, above which the field could be enhanced. In contrast to previously reported tapered structures in the adiabatic regime without transverse potentials, the structure proposed in this paper shows stronger focusing capability and allows monotonic increasing field enhancement over longer propagation distances.

Plasmonic black metals via radiation absorption by two-dimensional arrays of ultra-sharp convex grooves

Plasmonic black surfaces formed by two-dimensional arrays of ultra-sharp convex metal grooves, in which the incident radiation is converted into gap surface plasmon polaritons (GSPPs) and subsequently absorbed (via adiabatic nanofocusing), are fabricated and investigated experimentally for gold, nickel, and palladium, using scanning electron microscopy, optical microscopy, and reflection spectroscopy for their characterization. Absolute reflectivity spectra obtained for all fabricated arrays demonstrate very efficient and broadband absorption of unpolarized light exceeding the level of 95%, averaged over the investigated wavelength range of 400–985 nm. The highest averaged absorption level (~97%) is achieved with 250-nm-period arrays in palladium that also has the highest melting temperature (~1552°C), promising thereby potential applications for broadband absorption, e.g., within thermophotovoltaics. For one-dimensional arrays, GSPPs are excited only with the electric field polarized perpendicular to the groove orientation, resulting in 94–96% absorption of the appropriately polarized light for the arrays in nickel and palladium while featuring practically flat surface reflectivity spectra for the orthogonal polarization. The largest ratio (~10.7) between averaged reflectivities for orthogonal polarizations is achieved with the groove arrays in palladium, pointing thereby towards applications as broadband and low-dispersion linear polarizers operating in reflection, e.g., within ultra-fast optics.

Wave front adaptation using a deformable mirror for adiabatic nanofocusing along an ultrasharp gold taper

We describe and demonstrate the use of an adaptive wave front optimization scheme for enhancing the efficiency of adiabatic nanofocusing of surface plasmon polariton (SPP) waves along an ultrasharp conical gold taper. Adiabatic nanofocusing is an emerging and promising scheme for controlled focusing of far field light into nanometric volumes. It comprises three essential steps: SPP excitation by coupling far field light to an SPP waveguide, SPP propagation along the waveguide and adiabatic SPP nanofocusing towards a geometric singularity. For commonly used complex waveguide geometries, such as, e.g., conical metal tapers, a realistic modeling and efficiency optimization is challenging. Here, we use a deformable mirror to adaptively control the wave front of the incident far field light. We demonstrate an eight-fold enhancement in nanofocusing efficiency and analyze the shape of the resulting optimized wave front. The introduced wave front optimization scheme is of general interest for guiding and controlling light on the nanoscale.

K-space imaging of the eigenmodes of sharp gold tapers for scanning near-field optical microscopy

We investigate the radiation patterns of sharp conical gold tapers, which were designed as adiabatic nanofocusing probes for scanning near-field optical microscopy (SNOM). Field calculations show that only the lowest order eigenmode of such a taper can reach the very apex and thus induce the generation of strongly enhanced near-field signals. Higher-order modes are coupled into the far field at finite distances from the apex. Here, we demonstrate experimentally how to distinguish and separate between the lowest and higher-order eigenmodes of such a metallic taper by filtering in the spatial frequency domain. Our approach has the potential to considerably improve the signal-to-background ratio in spectroscopic experiments at the nanoscale.

Plasmonic black metals by broadband light absorption in ultra-sharp convex grooves

We have recently reported broadband (450–850 nm) and efficient (96% on average) light absorption on gold surfaces with arrays of ultra-sharp convex grooves via excitation and subsequent adiabatic nanofocusing and absorption of gap surface plasmon modes (Søndergaard et al 2012 Nature Commun. 3 969). Here, we significantly extend our spectroscopy investigations of one- and two-dimensional (1D and 2D) groove arrays in gold covering the wavelength range of 500–1700 nm and report first results on broadband light absorption by 1D groove arrays in nickel. For 1D groove arrays (periods 250 and 350 nm, groove depth 450 nm) in gold, the experimental characterization as well as numerical simulations based on the surface integral equation method reveal gradually increasing reflectivity for wavelengths above ∼650 nm reaching finally ∼60% at 1700 nm, but with a remarkable dip around 1150–1250 nm featuring only ∼10% reflectivity. Results indicate that the dip position can be adjusted with the precise groove geometry, a feature that could prove particularly useful for selective thermal emitters in thermophotovoltaics. Furthermore, investigations of field enhancement at the groove bottoms of 1D groove arrays in gold, mapped via diffraction-limited two-photon photoluminescence (TPL) scanning microscopy, reveal very selective polarization properties of excitation and TPL emission from the groove bottoms. 1D groove arrays in nickel were fabricated by making parallel 300 nm periodic adiabatic grooves of depths 100, 200, 300, 400 or 500 nm in a 600 nm thick nickel film. Their experimental characterization verifies that the structures are indeed very dark, exhibiting only 5–8% reflectivity over an entire wavelength range 400–1700 nm for the deepest grooves, which is in good correspondence with simulations.

Plasmonic black metals in resonant nanocavities

We investigate a plasmonic resonant structure tunable from ultra-violet to near infrared wavelengths with maximum absorbance strength over 95% due to a highly efficient coupling with incident light. Additional harmonics are excited at higher frequencies extending the absorbance range to multiple wavelengths. We propose the concept of a plasmonic black metal nanoresonator that exhibits broadband absorbance characteristics by spacing the modes closer through increasing the resonator length and by employing adiabatic plasmonic nano-focusing on the tapered end of the cavity.