On the theory of synchrotron radiation nanofocusing with planar compound refractive lenses.

Two new methods of computer simulation of synchrotron radiation nanofocusing with planar compound refractive lenses (PCRLs) are presented. The methods are based on the results of analytical theory. In contrast to previous works, the new methods take into account the PCRL aperture. It is especially important at high photon energies, when absorption is low and the calculations based on analytical theory, i.e. without taking into account the aperture, give incorrect results. A computer program was created and specific results were obtained for a silicon PCRL having an aperture of 50 µm, element length of 102 µm and minimum thickness of 2 µm. For an energy of 50 keV and number of elements 300, it focuses the beam to 31 nm size at a distance of one and a half times its length. Analysis of the calculation accuracy for the proposed methods is performed, as well as a demonstration of the capabilities of the computer program.

Feasibility of X-ray beam nanofocusing with compound refractive lenses.

A more general analytical theory of X-ray beam propagation through compound refractive lenses (CRLs) than the earlier study by Kohn [(2003). JETP, 97, 204-215] is presented. The problem of nanofocusing with CRLs is examined in detail. For a CRL with a relatively large aperture the focusing efficiency is limited by the radiation absorption in the lens material. The aperture does not affect the focusing process and it is replaced by the effective aperture. The X-ray transverse beam size at the focus is then by a factor of γ = ß/δ times smaller than the transverse beam size just behind the CRL. Here, δ and ß are the real and imaginary parts of the CRL material refractive index n = 1 - δ + iß. In this instance, to improve focusing efficiency, it is advantageous to decrease the CRL aperture and increase the photon energy E. However, with increasing photon energy, the material absorption decreases, which results in the CRL aperture impact on the transverse beam size. The latter leads to the fact that with a proper CRL length the beam size is independent of both the aperture and photon energy but depends only on the CRL material electron density and is approximately equal to wc = λ/(8δ)1/2, where λ denotes the radiation wavelength, as predicted by Bergemann et al. [(2003). Phys. Rev. Lett, 91, 204801].

Generation of an X-ray nanobeam of a free-electron laser using reflective optics with speckle interferometry.

Ultimate focusing of an X-ray free-electron laser (XFEL) enables the generation of ultrahigh-intensity X-ray pulses. Although sub-10 nm focusing has already been achieved using synchrotron light sources, the sub-10 nm focusing of XFEL beams remains difficult mainly because the insufficient stability of the light source hinders the evaluation of a focused beam profile. This problem is specifically disadvantageous for the Kirkpatrick-Baez (KB) mirror focusing system, in which a slight misalignment of ∼300 nrad can degrade the focused beam. In this work, an X-ray nanobeam of a free-electron laser was generated using reflective KB focusing optics combined with speckle interferometry. The speckle profiles generated by 2 nm platinum particles were systematically investigated on a single-shot basis by changing the alignment of the multilayer KB mirror system installed at the SPring-8 Angstrom Compact Free-Electron Laser, in combination with computer simulations. It was verified that the KB mirror alignments were optimized with the required accuracy, and a focused vertical beam of 5.8 nm (±1.2 nm) was achieved after optimization. The speckle interferometry reported in this study is expected to be an effective tool for optimizing the alignment of nano-focusing systems and for generating an unprecedented intensity of up to 1022 W cm-2 using XFEL sources.

X-Ray Single-Grating Interferometry for Wavefront Measurement and Correction of Hard X-Ray Nanofocusing Mirrors.

X-ray single-grating interferometry was applied to conduct accurate wavefront corrections for hard X-ray nanofocusing mirrors. Systematic errors in the interferometer, originating from a grating, a detector, and alignment errors of the components, were carefully examined. Based on the measured wavefront errors, the mirror shapes were directly corrected using a differential deposition technique. The corrected X-ray focusing mirrors with a numerical aperture of 0.01 attained two-dimensionally diffraction-limited performance. The results of the correction indicate that the uncertainty of the wavefront measurement was less than λ/72 in root-mean-square value.

X-ray mirror surface figure correction with nanometre precision controlled by layer stresses simulated by FEA.

Hard X-rays with energies higher than several kiloelectronvolts can be focused to spot sizes below 10 nm with the present synchrotron beamlines, offering unique advantages for the chemical, elemental and structure analysis of matter. Nevertheless, a surface precision on the nanometre scale for the focusing optics is required and remains the main hurdle limiting X-ray analytical techniques with single-nanometre spatial resolution. On the other hand, to preserve the wavefront properties of coherent X-ray beams, precise control of the reflective mirror surface quality at the nanometre scale is demanded for X-ray free-electron laser applications. In this work, the surface shape of a multilayer-coated X-ray mirror is controlled by layer stresses. The desired surface profile of the mirror is differentiated to its second order to obtain its corresponding curvature profile. With a step size of 1 mm along the mirror length, different coating thicknesses are applied to create different layer thermal stresses from uniform temperature change. The mirror surface profile can be obtained by integrating the curvature profile to its second order and further corrected by moving constant values for the slope and height. The technical process is simulated by finite element analysis (FEA). A case study showed that the residual slope error and the residual height error between the desired shape and the FEA result are 0.22 µrad (r.m.s.) and 1.42 nm (r.m.s.), respectively.

Selective Coherent Anti-Stokes Raman Scattering Microscopy Employing Dual-Wavelength Nanofocused Ultrafast Plasmon Pulses.

Ultrafast surface plasmon polariton (SPP) nanofocusing on a plasmonic metal tapered tip with femtosecond laser pulses enables background-free localized excitation beyond the diffraction limit. We demonstrate simultaneous nanofocusing of ultrafast SPP pulses at 440 and 800 nm, which were coupled with a common diffraction grating structure fabricated on an aluminum (Al) tapered tip, to the tip apex with a radius of ∼35 nm. We achieved selective coherent anti-Stokes Raman scattering (CARS) microscopy that combined an 800 nm (ω) SPP pump pulse, which achieves selective vibrational excitation by spectral focusing, and a 440 nm (2ω) SPP probe pulse. Raman intensity of this novel 2ω-CARS increased by a factor of 3.96 at the G-band and 4.00 at the 2D-band compared with that with ω-CARS for the monolayer graphene. The 2ω-CARS imaging method was applied for imaging a multiwalled carbon nanotube at the D-, G-, and 2D-bands. This dual-wavelength nanofocusing will open up new nanoscale microspectroscopy and optical excitation at the tip apex, such as sum frequency mixing, two-photon excitation.

Metamaterial Lensing Devices.

In recent years, the development of metamaterials and metasurfaces has drawn great attention, enabling many important practical applications. Focusing and lensing components are of extreme importance because of their significant potential practical applications in biological imaging, display, and nanolithography fabrication. Metafocusing devices using ultrathin structures (also known as metasurfaces) with superlensing performance are key building blocks for developing integrated optical components with ultrasmall dimensions. In this article, we review the metamaterial superlensing devices working in transmission mode from the perfect lens to two-dimensional metasurfaces and present their working principles. Then we summarize important practical applications of metasurfaces, such as plasmonic lithography, holography, and imaging. Different typical designs and their focusing performance are also discussed in detail.

Self-aligned deterministic coupling of single quantum emitter to nanofocused plasmonic modes.

The quantum plasmonics field has emerged and been growing increasingly, including study of single emitter-light coupling using plasmonic system and scalable quantum plasmonic circuit. This offers opportunity for the quantum control of light with compact device footprint. However, coupling of a single emitter to highly localized plasmonic mode with nanoscale precision remains an important challenge. Today, the spatial overlap between metallic structure and single emitter mostly relies either on chance or on advanced nanopositioning control. Here, we demonstrate deterministic coupling between three-dimensionally nanofocused plasmonic modes and single quantum dots (QDs) without any positioning for single QDs. By depositing a thin silver layer on a site-controlled pyramid QD wafer, three-dimensional plasmonic nanofocusing on each QD at the pyramid apex is geometrically achieved through the silver-coated pyramid facets. Enhancement of the QD spontaneous emission rate as high as 22 ± 16 is measured for all processed QDs emitting over ∼150-meV spectral range. This approach could apply to high fabrication yield on-chip devices for wide application fields, e.g., high-efficiency light-emitting devices and quantum information processing.

Aberration-free aspherical lens shape for shortening the focal distance of an already convergent beam.

The shapes of single lens surfaces capable of focusing divergent and collimated beams without aberration have already been calculated. However, nanofocusing compound refractive lenses (CRLs) require many consecutive lens surfaces. Here a theoretical example of an X-ray nanofocusing CRL with 48 consecutive surfaces is studied. The surfaces on the downstream end of this CRL accept X-rays that are already converging toward a focus, and refract them toward a new focal point that is closer to the surface. This case, so far missing from the literature, is treated here. The ideal surface for aberration-free focusing of a convergent incident beam is found by analytical computation and by ray tracing to be one sheet of a Cartesian oval. An `X-ray approximation' of the Cartesian oval is worked out for the case of small change in index of refraction across the lens surface. The paraxial approximation of this surface is described. These results will assist the development of large-aperture CRLs for nanofocusing.

Point focusing with flat and wedged crossed multilayer Laue lenses.

Point focusing measurements using pairs of directly bonded crossed multilayer Laue lenses (MLLs) are reported. Several flat and wedged MLLs have been fabricated out of a single deposition and assembled to realise point focusing devices. The wedged lenses have been manufactured by adding a stress layer onto flat lenses. Subsequent bending of the structure changes the relative orientation of the layer interfaces towards the stress-wedged geometry. The characterization at ESRF beamline ID13 at a photon energy of 10.5 keV demonstrated a nearly diffraction-limited focusing to a clean spot of 43 nm × 44 nm without significant side lobes with two wedged crossed MLLs using an illuminated aperture of approximately 17 µm × 17 µm to eliminate aberrations originating from layer placement errors in the full 52.7 µm × 52.7 µm aperture. These MLLs have an average individual diffraction efficiency of 44.5%. Scanning transmission X-ray microscopy measurements with convenient working distances were performed to demonstrate that the lenses are suitable for user experiments. Also discussed are the diffraction and focusing properties of crossed flat lenses made from the same deposition, which have been used as a reference. Here a focal spot size of 28 nm × 33 nm was achieved and significant side lobes were noticed at an illuminated aperture of approximately 23 µm × 23 µm.

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.

On-chip hybrid photonic-plasmonic light concentrator for nanofocusing in an integrated silicon photonics platform.

The enhancement and confinement of electromagnetic radiation to nanometer scale have improved the performances and decreased the dimensions of optical sources and detectors for several applications including spectroscopy, medical applications, and quantum information. Realization of on-chip nanofocusing devices compatible with silicon photonics platform adds a key functionality and provides opportunities for sensing, trapping, on-chip signal processing, and communications. Here, we discuss the design, fabrication, and experimental demonstration of light nanofocusing in a hybrid plasmonic-photonic nanotaper structure. We discuss the physical mechanisms behind the operation of this device, the coupling mechanisms, and how to engineer the energy transfer from a propagating guided mode to a trapped plasmonic mode at the apex of the plasmonic nanotaper with minimal radiation loss. Optical near-field measurements and Fourier modal analysis carried out using a near-field scanning optical microscope (NSOM) show a tight nanofocusing of light in this structure to an extremely small spot of 0.00563(λ/(2n(rmax)))(3) confined in 3D and an exquisite power input conversion of 92%. Our experiments also verify the mode selectivity of the device (low transmission of a TM-like input mode and high transmission of a TE-like input mode). A large field concentration factor (FCF) of about 4.9 is estimated from our NSOM measurement with a radius of curvature of about 20 nm at the apex of the nanotaper. The agreement between our theory and experimental results reveals helpful insights about the operation mechanism of the device, the interplay of the modes, and the gradual power transfer to the nanotaper apex.

Boosting Local Field Enhancement by on-Chip Nanofocusing and Impedance-Matched Plasmonic Antennas.

Strongly confined surface plasmon-polariton modes can be used for efficiently delivering the electromagnetic energy to nanosized volumes by reducing the cross sections of propagating modes far beyond the diffraction limit, that is, by nanofocusing. This process results in significant local-field enhancement that can advantageously be exploited in modern optical nanotechnologies, including signal processing, biochemical sensing, imaging, and spectroscopy. Here, we propose, analyze, and experimentally demonstrate on-chip nanofocusing followed by impedance-matched nanowire antenna excitation in the end-fire geometry at telecom wavelengths. Numerical and experimental evidence of the efficient excitation of dipole and quadrupole (dark) antenna modes are provided, revealing underlying physical mechanisms and analogies with the operation of plane-wave Fabry-Pérot interferometers. The unique combination of efficient nanofocusing and nanoantenna resonant excitation realized in our experiments offers a major boost to the field intensity enhancement up to ∼12000, with the enhanced field being evenly distributed over the gap volume of 30 × 30 × 10 nm(3), and promises thereby a variety of useful on-chip functionalities within sensing, nonlinear spectroscopy and signal processing.

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.

Nanofocusing of X-ray free-electron lasers by grazing-incidence reflective optics.

Total-reflection mirror devices for X-ray free-electron laser focusing are discussed in terms of optical design, mirror-fabrication technology, a wavefront diagnosis method and radiation-damage testing, as a review of the present status of the focusing optics at the SPring-8 angstrom compact free-electron laser (SACLA). Designed beam sizes of 1 µm and 50 nm, and spot sizes almost matching prediction have been achieved and used to explore topics at the forefront of natural science. The feasibility of these devices is determined to be sufficient for long-term and stable operation at SACLA by investigating the radiation-damage threshold and achievable accuracies in the mirror figure and alignment.

Sub-100 nm focusing of short wavelength plasmons in homogeneous 2D space.

We present a direct measurement of short-wavelength plasmons focused into a sub-100 nm spot in homogeneous (translation invariant) 2D space. The short-wavelength (SW) surface plasmon polaritons (SPP) are achieved in metal-insulator-insulator (MII) platform consisting of silver, silicon nitride, and air. This platform is homogeneous in two spatial directions and supports SPP at wavelength more than two times shorter than that in free space yet interacts with the outer world through the evanescent tail in air. We use an apertureless (scattering) near-field scanning optical microscope (NSOM) to map directly the amplitude and phase of these SW-SPP and show they can be focused to under 70 nm without structurally assisted confinement such as nanoantennas or nanofocusing. This, along with the use of visible light at 532 nm which is suitable for optical microscopy, can open new directions in direct biological and medical imaging at the sub-100 nm resolution regime.

Oxidation sharpening, template stripping, and passivation of ultra-sharp metallic pyramids and wedges.

Ultra-sharp metallic pyramids and wedges with tunable tip angles and 5-nm tip radii are replicated from oxidation-sharpened silicon templates with high throughput (80 million pyramids per wafer). Atomic layer deposition of Al2 O3 shells can protect these sharp pyramidal tips for subsequent usage in near-field imaging.

High-efficiency zone-plate optics for multi-keV X-ray focusing.

High-efficiency nanofocusing of hard X-rays using stacked multilevel Fresnel zone plates with a smallest zone width of 200 nm is demonstrated. The approach is to approximate the ideal parabolic lens profile with two-, three-, four- and six-level zone plates. By stacking binary and three-level zone plates with an additional binary zone plate, the number of levels in the optical transmission function was doubled, resulting in four- and six-level profiles, respectively. Efficiencies up to 53.7% focusing were experimentally obtained with 6.5 keV photons using a compact alignment apparatus based on piezoelectric actuators. The measurements have also been compared with numerical simulations to study the misalignment of the two zone plates.

Ptychography with multilayer Laue lenses.

Two different multilayer Laue lens designs were made with total deposition thicknesses of 48 µm and 53 µm, and focal lengths of 20.0 mm and 12.5 mm at 20.0 keV, respectively. From these two multilayer systems, several lenses were manufactured for one- and two-dimensional focusing. The latter is realised with a directly bonded assembly of two crossed lenses, that reduces the distance between the lenses in the beam direction to 30 µm and eliminates the necessity of producing different multilayer systems. Characterization of lens fabrication was performed using a laboratory X-ray microscope. Focusing properties have been investigated using ptychography.

Metallic On-Chip Light Concentrators Fabricated by In Situ Plasmonic Etching Technique.

One-dimensional tapered metallic nanostructures are highly interesting for nanophotonic applications because of their plasmonic waveguiding and field-focusing properties. Here, we developed an in situ etching technique for unique tapered crystallized silver nanowire fabrication. Under the focused laser spot, plasmon-induced charge separation of chemically synthesized nanowires is excited, which triggers the uniaxial etching of silver nanowires along the radial direction with decreasing rate, forming tapered structures several micrometers long and with diameter attenuating from hundreds to tens of nanometers. These tapered metallic nanowires have smooth surfaces showing excellent performance for plasmonic waveguiding, and can be good candidates for nanocircuits and remote-excitation sources.