High-speed fixed-target serial virus crystallography.

We report a method for serial X-ray crystallography at X-ray free-electron lasers (XFELs), which allows for full use of the current 120-Hz repetition rate of the Linear Coherent Light Source (LCLS). Using a micropatterned silicon chip in combination with the high-speed Roadrunner goniometer for sample delivery, we were able to determine the crystal structures of the picornavirus bovine enterovirus 2 (BEV2) and the cytoplasmic polyhedrosis virus type 18 polyhedrin, with total data collection times of less than 14 and 10 min, respectively. Our method requires only micrograms of sample and should therefore broaden the applicability of serial femtosecond crystallography to challenging projects for which only limited sample amounts are available. By synchronizing the sample exchange to the XFEL repetition rate, our method allows for most efficient use of the limited beam time available at XFELs and should enable a substantial increase in sample throughput at these facilities.

Less Is More: Enhancement of Second-Harmonic Generation from Metasurfaces by Reduced Nanoparticle Density.

We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to expectations, a substantial enhancement of the SHG signal is observed when the number density of the particles in the array is reduced. More specifically, by halving the number density, we obtain over 5-fold enhancement in SHG intensity. This striking result is attributed to favorable interparticle interactions mediated by the lattice, where surface-lattice resonances lead to spectral narrowing of the plasmon resonances. Importantly, however, the results cannot be explained by the improved quality of the plasmon resonance alone. Instead, the lattice interactions also lead to further enhancement of the local fields at the particles. The experimental observations agree very well with results obtained from numerical simulations including lattice interactions.

Comparison of metal/polymer back reflectors with half-sphere, blazed, and pyramid gratings for light trapping in III-V solar cells.

We report on the fabrication of diffraction gratings for application as back contact reflectors. The gratings are designed for thin-film solar cells incorporating absorbers with bandgap slightly lower than GaAs, i.e. InAs quantum dot or GaInNAs solar cells. Light trapping in the solar cells enables the increase of the absorption leading to higher short circuit current densities and higher efficiencies. We study metal/polymer back reflectors with half-sphere, blazed, and pyramid gratings, which were fabricated either by photolithography or by nanoimprint lithography. The gratings are compared in terms of the total and the specular reflectance, which determine their diffraction capabilities, i.e. the feature responsible for increasing the absorption. The pyramid grating showed the highest diffuse reflection of light compared to the half-sphere structure and the blazed grating. The diffraction efficiency measurements were in agreement with the numerical simulations. The validated model enables designing such metal/polymer back reflectors for other type of solar cells by refining the optimal dimensions of the gratings for different wavelength ranges.

Strip-loaded horizontal slot waveguide.

We introduce a novel concept for an optical waveguide called a strip-loaded slot waveguide. It allows an extraordinary confinement of the field in a waveguide with an extremely tiny (vertical) cross section. Unlike conventional slot waveguides, the proposed configuration has potential for very low propagation losses. Its operation is demonstrated at telecommunication wavelengths and, in addition, it is fabricated by means of mass production compatible techniques: atomic layer deposition and nanoimprint replication. The possibility to fabricate the proposed structure with such low-cost techniques opens a new path for a variety of nanophotonics applications.

Surface Plasmons Carry the Pancharatnam-Berry Geometric Phase.

Surface plasmon polaritons (SPPs) are electromagnetic surface waves that travel along the boundary of a metal and a dielectric medium. They can be generated when freely propagating light is scattered by structural metallic features such as gratings or slits. In plasmonics, SPPs are manipulated, amplified, or routed before being converted back into light by a second scattering event. In this process, the light acquires a dynamic phase and perhaps an additional geometric phase associated with polarization changes. We examine the possibility that SPPs mediate the Pancharatnam-Berry phase, which follows from a closed path of successive in-phase polarization-state transformations on the Poincaré sphere and demonstrate that this is indeed the case. The geometric phase is shown to survive the light→SPP→light process and, moreover, its magnitude agrees with Pancharatnam's rule. Our findings are fundamental in nature and highly relevant for photonics applications.

Quasi-monochromatic modes of quasi-stationary, pulsed scalar optical fields.

We investigate the temporal coherence of random, pulsed, quasi-stationary scalar light fields and introduce a new type of expansion for the mutual coherence function in terms of fully coherent frequency-shifted quasi-monochromatic modes of identical shape. The mode representation is valid provided the pulse length is shorter and the coherence time is much shorter than the width of the time window in which the field is considered. The construction of the expansion is particularly straightforward since information is required only on the average spectrum and the average temporal intensity. The method enables us to assess the coherence properties of quasi-stationary light by analyzing the behavior of deterministic quasi-monochromatic fields. The frequency-domain counterpart of the representation is also given. The method is illustrated by application to a pulsed free-electron laser source.

Dielectric V-ridge gratings: transition from antireflection to retroreflection.

We present a systematic study of the optical properties of dielectric gratings with symmetric V-shaped ridges having a 90 degree apex angle and refractive index n. Such structures exhibit completely different optical properties if the dimensions are scaled with respect to the vacuum wavelength λ0 of light. In the subwavelength domain, where the grating period d is less than λ0/n, the grating behaves as an antireflection layer. In the large-period domain d≫λ0 (with normal incidence from the dielectric side), the grating turns into a micro-retroreflector array. The transition between these well-known domains is studied using rigorous diffraction theory. The results are verified experimentally by fabricating and characterizing V-profile gratings with the aid of wet etching of silicon using a process that defines a 90 degree apex angle and replication into a polymer.

Add-drop filter based on TiO2 coated shifted Bragg grating.

We present a titanium dioxide coated shifted Bragg grating in a silicon-on-insulator platform enabling optical add-drop functionality. The device works on the basis of mode conversion due to shifted sidewall structure followed by mode splitting based on an asymmetric Y-coupler. We experimentally demonstrate the working principle of the device. A reflection bandwidth of 2.2 nm with 14 dB extinction ratio is obtained with a 300 µm long shifted Bragg grating. The performance of the device is also compared without the titanium dioxide coating. A scope of spectral tunability with titanium dioxide re-coating (0.8 nm per 1 nm re-coating) by atomic layer deposition is experimentally verified.

On spectral and temporal coherence of x-ray free-electron laser beams.

A model for the coherence properties of free-electron lasers (FELs) in time and frequency domains is introduced within the framework of classical second-order coherence theory of nonstationary light. An iterative phase-retrieval algorithm is applied to construct an ensemble of field realizations in both domains, based on single-pulse spectra measured at the Linac Coherent Light Source (LCLS) in self-amplified spontaneous emission mode. Such an ensemble describes the specific FEL pulse train in a statistically averaged sense. Two-time and two-frequency correlation functions are constructed, demonstrating that the hard X-ray free-electron laser at LCLS in this case behaves as a quasistationary source with low spectral and temporal coherence. We also show that the Gaussian Schell model provides a good description of this FEL.

Zernike x-ray ptychography.

We present an imaging technique combining Zernike phase-contrast imaging and ptychography. The contrast formation is explained by following the theory of Zernike phase-contrast imaging. The method is demonstrated with x-rays at a photon energy of 6.2 keV, showing how ptychographic reconstruction of a phase sample leads to a Zernike phase-contrast image appearing in the amplitude reconstruction. In addition, the results presented in this Letter indicate an improvement of the resolution of the reconstructed object in the case of Zernike ptychography compared with the conventional one.

Fabrication and characterization of high-efficiency double-sided blazed x-ray optics.

The focusing efficiency of conventional diffractive x-ray lenses is fundamentally limited due to their symmetric binary structures and the corresponding symmetry of their focusing and defocusing diffraction orders. Fresnel zone plates with asymmetric structure profiles can break this limitation; yet existing implementations compromise either on resolution, ease of use, or stability. We present a new way for the fabrication of such blazed lenses by patterning two complementary binary Fresnel zone plates on the front and back sides of the same membrane chip to provide a compact, inherently stable, single-chip device. The presented blazed double-sided zone plates with 200 nm smallest half-pitch provide up to 54.7% focusing efficiency at 6.2 keV, which is clearly beyond the value obtainable by their binary counterparts.

Artifact characterization and reduction in scanning X-ray Zernike phase contrast microscopy.

Zernike phase contrast microscopy is a well-established method for imaging specimens with low absorption contrast. It has been successfully implemented in full-field microscopy using visible light and X-rays. In microscopy Cowley's reciprocity principle connects scanning and full-field imaging. Even though the reciprocity in Zernike phase contrast has been discussed by several authors over the past thirty years, only recently it was experimentally verified using scanning X-ray microscopy. In this paper, we investigate the image and contrast formation in scanning Zernike phase contrast microscopy with a particular and detailed focus on the origin of imaging artifacts that are typically associated with Zernike phase contrast. We demonstrate experimentally with X-rays the effect of the phase mask design on the contrast and halo artifacts and present an optimized design of the phase mask with respect to photon efficiency and artifact reduction. Similarly, due to the principle of reciprocity the observations and conclusions of this work have direct applicability to Zernike phase contrast in full-field microscopy as well.

High resolution double-sided diffractive optics for hard X-ray microscopy.

The fabrication of high aspect ratio metallic nanostructures is crucial for the production of efficient diffractive X-ray optics in the hard X-ray range. We present a novel method to increase their structure height via the double-sided patterning of the support membrane. In transmission, the two Fresnel zone plates on the two sides of the substrate will act as a single zone plate with added structure height. The presented double-sided zone plates with 30 nm smallest zone width offer up to 9.9% focusing efficiency at 9 keV, that results in a factor of two improvement over their previously demonstrated single-sided counterparts. The increase in efficiency paves the way to speed up X-ray microscopy measurements and allows the more efficient utilization of the flux in full-field X-ray microscopy.

Element-specific X-ray phase tomography of 3D structures at the nanoscale.

Recent advances in fabrication techniques to create mesoscopic 3D structures have led to significant developments in a variety of fields including biology, photonics, and magnetism. Further progress in these areas benefits from their full quantitative and structural characterization. We present resonant ptychographic tomography, combining quantitative hard x-ray phase imaging and resonant elastic scattering to achieve ab initio element-specific 3D characterization of a cobalt-coated artificial buckyball polymer scaffold at the nanoscale. By performing ptychographic x-ray tomography at and far from the Co K edge, we are able to locate and quantify the Co layer in our sample to a 3D spatial resolution of 25 nm. With a quantitative determination of the electron density we can determine that the Co layer is oxidized, which is confirmed with microfluorescence experiments.

Towards tender X-rays with Zernike phase-contrast imaging of biological samples at 50 nm resolution.

X-ray microscopy is a commonly used method especially in material science application, where the large penetration depth of X-rays is necessary for three-dimensional structural studies of thick specimens with high-Z elements. In this paper it is shown that full-field X-ray microscopy at 6.2 keV can be utilized for imaging of biological specimens with high resolution. A full-field Zernike phase-contrast microscope based on diffractive optics is used to study lipid droplet formation in hepatoma cells. It is shown that the contrast of the images is comparable with that of electron microscopy, and even better contrast at tender X-ray energies between 2.5 keV and 4 keV is expected.

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.

Halo suppression in full-field x-ray Zernike phase contrast microscopy.

Visible light Zernike phase contrast (ZPC) microscopy is a well established method for imaging weakly absorbing samples. The method is also used with hard x-ray photon energies for structural evaluation of material science and biological applications. However, the method suffers from artifacts that are inherent for the Zernike image formation. In this Letter, we investigate their origin and experimentally show how to suppress them in x-ray full-field ZPC microscopy based on diffractive x-ray optics.

Coherence-polarization mixing in resonance gratings.

We show, using rigorous diffraction theory, that resonance gratings can be used to transfer partial spatial correlation to partial polarization even if the incident light beam is fully polarized. The phenomenon is based on the fact that either of the two orthogonal polarization components can be coupled into the leaky waveguide mode, leading to a strong phase delay, while the other one is reflected without being coupled into the grating. Numerical demonstrations are based on a Gaussian Schell-model beam and a grating analysis performed by rigorous Fourier modal method.

Enhanced dual-band infrared absorption in a Fabry-Perot cavity with subwavelength metallic grating.

The performance of infrared (IR) dual-band detector can be substantially improved by simultaneously increasing IR absorptions for both sensor bands. Currently available methods only provide absorption enhancement for single spectral band, but not for the dual-band. The Fabry-Perot (FP) cavity generates a series of resonances in multispectral bands. With this flexibility, we introduced a novel type of dual-band detector structure containing a multilayer FP cavity with two absorbing layers and a subwavelength-period grating mirror, which is capable of simultaneously enhancing the middle wave infrared (MWIR) and the long wave infrared (LWIR) detection. Compared with the bare-absorption-layer detector (common dual-band detector), the optimized FP cavity can provide about 13 times and 17 times absorption enhancement in LWIR and MWIR bands respectively.

Resonance waveguide reflectors with semi-wide bandwidth at the visible wavelengths.

We present a resonance waveguide grating with relatively wide bandwidth in the visible region of the spectrum compared to typical resonance structures. The reflective properties of the grating are based on amorphous atomic layer deposited titanium dioxide which has rather high refractive index at the visible wavelengths. The resonance grating provides approximately 20-30 nm bandwidth with over 90% reflectance at the visible wavelengths. The measured reflectances of the fabricated elements show also very good agreement with the theoretical predictions. These kind of reflectors may be useful in applications that make use of LED sources.