Slope error correction on X-ray reflection gratings by a variation of the local line density.

The patterning of x-ray grating surfaces by electron-beam lithography offers large flexibility to realize complex optical functionalities. Here, we report on a proof-of-principle experiment to demonstrate the correction of slope errors of the substrates by modulating the local density of the grating lines. A surface error map of a test substrate was determined by optical metrology and served as the basis for an aligned exposure of a corrected grating pattern made by electron-beam lithography. The correction is done by a variation of the local line density in order to compensate for the local surface error. Measurements with synchrotron radiation and simulations in the soft X-ray range confirm that the effects of slope errors were strongly reduced over an extended wavelength range.

Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

Metal assisted chemical etching of silicon in the gas phase: a nanofabrication platform for X-ray optics.

High aspect ratio nanostructuring requires high precision pattern transfer with highly directional etching. In this work, we demonstrate the fabrication of structures with ultra-high aspect ratios (up to 10 000 : 1) in the nanoscale regime (down to 10 nm) by platinum assisted chemical etching of silicon in the gas phase. The etching gas is created by a vapour of water diluted hydrofluoric acid and a continuous air flow, which works both as an oxidizer and as a gas carrier for reactive species. The high reactivity of platinum as a catalyst and the formation of platinum silicide to improve the stability of the catalyst pattern allow a controlled etching. The method has been successfully applied to produce straight nanowires with section size in the range of 10-100 nm and length of hundreds of micrometres, and X-ray optical elements with feature sizes down to 10 nm and etching depth in the range of tens of micrometres. This work opens the possibility of a low cost etching method for stiction-sensitive nanostructures and a large range of applications where silicon high aspect ratio nanostructures and high precision of pattern transfer are required.

A zone-plate-based two-color spectrometer for indirect X-ray absorption spectroscopy.

X-ray absorption spectroscopy (XAS) is a powerful element-specific technique that allows the study of structural and chemical properties of matter. Often an indirect method is used to access the X-ray absorption (XA). This work demonstrates a new XAS implementation that is based on off-axis transmission Fresnel zone plates to obtain the XA spectrum of La0.6Sr0.4MnO3 by analysis of three emission lines simultaneously at the detector, namely the O 2p-1s, Mn 3s-2p and Mn 3d-2p transitions. This scheme allows the simultaneous measurement of an integrated total fluorescence yield and the partial fluorescence yields (PFY) of the Mn 3s-2p and Mn 3d-2p transitions when scanning the Mn L-edge. In addition to this, the reduction in O fluorescence provides another measure for absorption often referred to as the inverse partial fluorescence yield (IPFY). Among these different methods to measure XA, the Mn 3s PFY and IPFY deviate the least from the true XA spectra due to the negligible influence of selection rules on the decay channel. Other advantages of this new scheme are the potential to strongly increase the efficiency and throughput compared with similar measurements using conventional gratings and to increase the signal-to-noise of the XA spectra as compared with a photodiode. The ability to record undistorted bulk XA spectra at high flux is crucial for future in situ spectroscopy experiments on complex materials.

High-intensity x-ray microbeam for macromolecular crystallography using silicon kinoform diffractive lenses.

Macromolecular crystallography often requires focused high-intensity x-ray beams for solving challenging protein structures from micrometer-sized crystals using current synchrotron radiation sources. The design of optical focusing schemes for hard x-rays showing high efficiency and flexibility in beam size is therefore continuously pursued. Here, we present an innovative solution based on a two-stage demagnification of the undulator source for photon energies from 6 keV to 19 keV, commissioned at the X10SA beamline of the Swiss Light Source, where a secondary source is imaged by two crossed silicon kinoform x-ray diffractive lenses with 75 nm outermost zone width. A source-size limited spot with a size of 4.8 µm×1.7 µm(h×v,FWHM) and flux of 7.5×1010 photons/s at 12.4 keV is demonstrated at the sample position.

High-acceptance versatile microfocus module based on elliptical Fresnel zone plates for small-angle X-ray scattering.

High-efficiency microfocusing of multi-keV X-rays at synchrotron sources is highly profitable for spatially resolved structural analysis of many kinds. Because radiation from synchrotron sources is typically elongated along the horizontal dimension, generating a microbeam that is isotropic in size requires a carefully designed optics system. Here we report on using a combination of a horizontally tunable slit downstream of the undulator source with elliptical diffractive Fresnel zone plates. We demonstrate the arrangement in context of small-angle X-ray scattering experiments, obtaining a microbeam of 2.2 µm × 1.8 µm (X × Y) with a flux of 1.2 × 1010 photons/s at an energy of 11.2 keV at the sample position.

Transmission zone plates as analyzers for efficient parallel 2D RIXS-mapping.

We have implemented and successfully tested an off-axis transmission Fresnel zone plate as spectral analyzer for resonant inelastic X-ray scattering (RIXS). The imaging capabilities of zone plates allow for advanced two-dimensional (2D) mapping applications. By varying the photon energy along a line focus on the sample, we were able to simultaneously record the emission spectra over a range of excitation energies. Moreover, by scanning a line focus across the sample in one dimension, we efficiently recorded RIXS spectra spatially resolved in 2D, increasing the throughput by two orders of magnitude. The presented scheme opens up a variety of novel measurements and efficient, ultra-fast time resolved investigations at X-ray Free-Electron Laser sources.

Zone plates as imaging analyzers for resonant inelastic x-ray scattering.

We have implemented and successfully tested an off-axis transmission Fresnel zone plate as a novel type of analyzer optics for resonant inelastic x-ray scattering (RIXS). We achieved a spectral resolution of 64 meV at the nitrogen K-edge (E/dE = 6200), closely matching theoretical predictions. The fundamental advantage of transmission optics is the fact that it can provide stigmatic imaging properties. This opens up a variety of advanced RIXS configurations, such as efficient scanning RIXS, parallel detection for varying incident energy and time-resolved measurements.

Electron-Beam Lithographic Grafting of Functional Polymer Structures from Fluoropolymer Substrates.

Well-defined submicrometer structures of poly(dimethylaminoethyl methacrylate) (PDMAEMA) were grafted from 100 µm thick films of poly(ethene-alt-tetrafluoroethene) after electron-beam lithographic exposure. To explore the possibilities and limits of the method under different exposure conditions, two different acceleration voltages (2.5 and 100 keV) were employed. First, the influence of electron energy and dose on the extent of grafting and on the structure's morphology was determined via atomic force microscopy. The surface grafting with PDMAEMA was confirmed by advanced surface analytical techniques such as time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy. Additionally, the possibility of effective postpolymerization modification of grafted structures was demonstrated by quaternization of the grafted PDMAEMA to the polycationic QPDMAEMA form and by exploiting electrostatic interactions to bind charged organic dyes and functional proteins.

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.

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.

Multiple scattering tomography.

Multiple scattering represents a challenge for numerous modern tomographic imaging techniques. In this Letter, we derive an appropriate line integral that allows for the tomographic reconstruction of angular resolved scattering distributions, even in the presence of multiple scattering. The line integral is applicable to a wide range of imaging techniques utilizing various kinds of probes. Here, we use x-ray grating interferometry to experimentally validate the framework and to demonstrate additional structural sensitivity, which exemplifies the impact of multiple scattering tomography.

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.

Novel 3D micro- and nanofabrication method using thermally activated selective topography equilibration (TASTE) of polymers.

Micro- and nanostructures with three-dimensional (3D) shapes are needed for a variety of applications in optics and fluidics where structures with both smooth and sharp features enhance the performance and functionality. We present a novel method for the generation of true 3D surfaces based on thermally activated selective topography equilibration (TASTE). This technique allows generating almost arbitrary sloped, convex and concave profiles in the same polymer film with dimensions in micro- and nanometer scale. We describe its principal mechanism exemplified by pre-patterned poly (methyl methacrylate) resist which is exposed to high energy electrons prior to a thermal annealing step enabling the selective transformation of stepped contours into smooth surfaces. From this we conclude, that TASTE not only offers an enormous degree of freedom for future process variations, but also will advance the patterning capabilities of current standard 3D micro- and nanofabrication methods.

A sensitive x-ray phase contrast technique for rapid imaging using a single phase grid analyzer.

Phase contrast x-ray imaging (PCXI) is a promising imaging modality, capable of sensitively differentiating soft tissue structures at high spatial resolution. However, high sensitivity often comes at the cost of a long exposure time or multiple exposures per image, limiting the imaging speed and possibly increasing the radiation dose. Here, we demonstrate a PCXI method that uses a single short exposure to sensitively capture sample phase information, permitting high speed x-ray movies and live animal imaging. The method illuminates a checkerboard phase grid to produce a fine grid-like intensity reference pattern at the detector, then spatially maps sample-induced distortions of this pattern to recover differential phase images of the sample. The use of a phase grid is an improvement on our previous absorption grid work in two ways. There is minimal loss in x-ray flux, permitting faster imaging, and, a very fine pattern is produced for homogenous high spatial resolution. We describe how this pattern permits retrieval of five images from a single exposure; the sample phase gradient images in the horizontal and vertical directions, a projected phase depth image, an edge-enhanced image, and a type of scattering image. Finally, we describe how the reconstruction technique can achieve subpixel distortion retrieval and study the behavior of the technique in regard to analysis technique, Talbot distance, and exposure time.

Understanding the electrolyte background for biochemical sensing with ion-sensitive field-effect transistors.

Silicon nanowire field-effect transistors have attracted substantial interest for various biochemical sensing applications, yet there remains uncertainty concerning their response to changes in the supporting electrolyte concentration. In this study, we use silicon nanowires coated with highly pH-sensitive hafnium oxide (HfO(2)) and aluminum oxide (Al(2)O(3)) to determine their response to variations in KCl concentration at several constant pH values. We observe a nonlinear sensor response as a function of ionic strength, which is independent of the pH value. Our results suggest that the signal is caused by the adsorption of anions (Cl(-)) rather than cations (K(+)) on both oxide surfaces. By comparing the data to three well-established models, we have found that none of those can explain the present data set. Finally, we propose a new model which gives excellent quantitative agreement with the data.

Generation of extreme ultraviolet vortex beams using computer generated holograms.

We fabricate computer generated holograms for the generation of phase singularities at extreme ultraviolet (EUV) wavelengths using electron beam lithography and demonstrate their ability to generate optical vortices in the nonzero diffraction orders. To this end, we observe the characteristic intensity distribution of the vortex beam and verify the helical phase structure interferometrically. The presented method forms the basis for further studies on singular light fields in the EUV frequency range, i.e., in EUV interference lithography. Since the method is purely achromatic, it may also find applications in various fields of x ray optics.

High-efficiency Fresnel zone plates for hard X-rays by 100 keV e-beam lithography and electroplating.

The fabrication and characterization of Fresnel zone plates (FZPs) for hard X-ray microscopy applications are reported. High-quality 500 nm- and 1 µm-thick Au FZPs with outermost zone widths down to 50 nm and 70 nm, respectively, and with diameters up to 600 µm were fabricated. The diffraction efficiencies of the fabricated FZPs were measured for a wide range of X-ray energies (2.8-13.2 keV) showing excellent values up to 65-75% of the theoretical values, reflecting the good quality of the FZPs. Spatially resolved diffraction efficiency measurements indicate the uniformity of the FZPs and a defect-free structure.

Ultra-high resolution zone-doubled diffractive X-ray optics for the multi-keV regime.

X-ray microscopy based on Fresnel zone plates is a powerful technique for sub-100 nm resolution imaging of biological and inorganic materials. Here, we report on the modeling, fabrication and characterization of zone-doubled Fresnel zone plates for the multi-keV regime (4-12 keV). We demonstrate unprecedented spatial resolution by resolving 15 nm lines and spaces in scanning transmission X-ray microscopy, and focusing diffraction efficiencies of 7.5% at 6.2 keV photon energy. These developments represent a significant step towards 10 nm spatial resolution for hard X-ray energies of up to 12 keV.

Titania-assisted electron-beam and synchrotron lithography.

Novel imaging layer technology for electron-beam and extreme-ultraviolet lithographic processes based upon generation of Pd nanoparticles in the Pd(2+)-loaded TiO(2) films was developed. The electroless metallization of the patterned TiO(2):Pd(2+) films yields both negative and positive nickel images with resolution down to approximately 100 nm.