Reflection Zone Plates Research Articles

High‐resolution x‐ray emission spectrometry in the lithium K range with a reflection zone plate spectrometer

AbstractImplementing a newly developed spectrometer for the soft x‐ray range of (35–130) eV based on reflection zone plates was successfully accomplished on an electron probe microanalyzer. In this context, we present the first spectra acquired using this setup, including those of elements such as Be (Kα), C (Kα), Mg (L2,3), Al (L2,3), and Si (L2,3). We have also conducted an analysis of several lithium compounds and measured the emission of Li Kα from metallic Li, LiF, and LiNbO3. Some of the results were compared with density functional theory calculations. The spectrum obtained for the lithium‐bearing mineral amblygonite Li0.75Na0.25Al(PO4)F0.75(OH)0.25 is chosen to discuss some of the challenges faced.

Performance analysis of single-focus phase singularity based on elliptical reflective annulus quadrangle-element coded spiral zone plates

Optical vortices generated by the conventional vortex lens are usually disturbed by the undesired higher-order foci, which may lead to additional artifacts and thus degrade the contrast sensitivity. In this work, we propose an efficient methodology to combine the merit of elliptical reflective zone plates (ERZPs) and the advantage of spiral zone plates (SZPs) in establishing a specific single optical element, termed elliptical reflective annulus quadrangle-element coded spiral zone plates (ERAQSZPs) to generate single-focus phase singularity. Differing from the abrupt reflectance of the ERZPs, a series of randomly distributed nanometer apertures are adopted to realize the sinusoidal reflectance. Typically, according to our physical design, the ERAQSZPs are fabricated on a bulk substrate; therefore, the new idea can significantly reduce the difficulty in the fabrication process. Based on the Kirchhoff diffraction theory and convolution theorem, the focusing performance of ERAQSZPs is calculated. The results reveal that apart from the capability of generating optical vortices, ERAQSZPs can also integrate the function of focusing, energy selection, higher-order foci elimination, as well as high spectral resolution together. In addition, the focusing properties can be further improved by appropriately adjusting the parameters, such as zone number and the size of the consisted primitives. These findings are expected to direct a new direction toward improving the performance of optical capture, x-ray fluorescence spectra, and forbidden transition.

Versatile tabletop setup for picosecond time-resolved resonant soft-x-ray scattering and spectroscopy.

We present a laser-driven, bright, and broadband (50 to 1500eV) soft-x-ray plasma source with <10ps pulse duration. This source is employed in two complementary, laboratory-scale beamlines for time-resolved, magnetic resonant scattering and spectroscopy, as well as near-edge x-ray absorption fine-structure (NEXAFS) spectroscopy. In both beamlines, dedicated reflection zone plates (RZPs) are used as single optical elements to capture, disperse, and focus the soft x rays, reaching resolving powers up to E/ΔE > 1000, with hybrid RZPs at the NEXAFS beamline retaining a consistent E/ΔE > 500 throughout the full spectral range, allowing for time-efficient data acquisition. We demonstrate the versatility and performance of our setup by a selection of soft-x-ray spectroscopy and scattering experiments, which so far have not been possible on a laboratory scale. Excellent data quality, combined with experimental flexibility, renders our approach a true alternative to large-scale facilities, such as synchrotron-radiation sources and free-electron lasers.

Dual-band and dual-polarized reflective Fresnel zone plate design based on Fractal shape

In this study, a dual-polarized and dual band reflective Fresnel zone plate with reconfigurable beam is proposed on the basis of fractal frequency selective surface (FSS) unit with nearly 360° phase tunability. Firstly, a new phase distribution calculation strategy based on Fresnel diffraction theory is proposed to improve the performance under certain scenarios like sparse arrays. Then, a novel fractal shape is put forward and applied to the design of the Fresnel zone plate. The introduction of the fractal structure makes the unit cell perform dual band, dual polarization and 309° phase tunability characteristics. Due to the self-symmetry of the unit cell, the proposed fractal Fresnel zone plate (FFZP) is capable of beam steering in ± 45° in both TE and TM incident waves. Besides, the proposed structure shows small performance degradation when it comes to oblique incidence up to 45°, which decreases the focal diameter ratio and profile of the proposed FFZP. The operating bandwidth of the FFZP can reach up to 700 MHz at X and Ku bands. It is applicable in a wide range of RF and microwave settings such as satellite and base station.

Advancements in Liquid Jet Technology and X-ray Spectroscopy for Understanding Energy Conversion Materials during Operation.

ConspectusWater splitting is intensively studied for sustainable and effective energy storage in green/alternative energy harvesting-storage-release cycles. In this work, we present our recent developments for combining liquid jet microtechnology with different types of soft X-ray spectroscopy at high-flux X-ray sources, in particular developed for studying the oxygen evolution reaction (OER). We are particularly interested in the development of in situ photon-in/photon-out techniques, such as in situ resonant inelastic X-ray scattering (RIXS) techniques at high-repetition-frequency X-ray sources, pointing toward operando capabilities. The pilot catalytic systems we use are perovskites having the general structure ABO3 with lanthanides or group II elements at the A sites and transition metals at the B sites. Depending on the chemical substitutions of ABO3, their catalytic activity for OER can be tuned by varying the composition.In this work, we present our in situ RIXS studies of the manganese L-edge of perovskites during OER. We have developed various X-ray spectroscopy approaches like transmission zone plate-, reflection zone plate-, and grating-based emission spectroscopy techniques. Combined with tunable incident X-ray energies, we yield complementary information about changing (inverse) X-ray absorption features of the perovskites, allowing us to deduce element- and oxidation-state-specific chemical monitoring of the catalyst. Adding liquid jet technology, we monitor element- and oxidation-state-specific interactions of the catalyst with water adsorbate during OER. By comparing the different technical spectroscopy approaches combined with high-repetition-frequency experiments at synchrotrons and free-electron lasers, we conclude that the combination of liquid jet with low-resolution zone-plate-based X-ray spectroscopy is sufficient for element- and oxidation-state-specific chemical monitoring during OER and easy to handle.For an in-depth study of OER mechanisms, however, including the characterization of catalyst-water adsorbate in terms of their charge transfer properties and especially valence intermediates formed during OER, high-resolution spectroscopy tools based on a combination of liquid jets with gratings bear bigger potential since they allow resolution of otherwise-overlapping X-ray spectroscopy transitions. Common for all of these experimental approaches is the conclusion that without the versatile developments of liquid jets and liquid beam technologies, elaborate experiments such as high-repetition experiments at high-flux X-ray sources (like synchrotrons or free-electron lasers) would hardly be possible. Such experiments allow sample refreshment for every single X-ray shot for repetition frequencies of up to 5 MHz, so that it is possible (a) to study X-ray-radiation-sensitive samples and also (b) to utilize novel types of flux-hungry X-ray spectroscopy tools like photon-in/photon-out X-ray spectroscopy to study the OER.

Broadband Time-Delay and Chirp Compensator for X-ray Pulses

A new type of aberration-corrected time-delay compensating monochromator (TDCM) for soft X-rays is presented. Composed of two identical reflection zone plates (RZPs) on spherical substrates and an intermediate flat mirror for band-pass selection, the TDCM can operate in a wide energy range of about ±20% around the design energy of 410eV. Assuming a source size of 50μm and an angular acceptance of 1 mrad, the spectral resolving power may reach 6×102, at a pulse length as short as 4.3femtoseconds(fs). In the case of μm-sized sources, the resolution can be better than 0.1eV and the sub-fs regime could become accessible. The overall transmission efficiency varies within (4.2–6.0)% across the energy range (310–510) eV. In the complementary mode, chirped-pulse compression works as well. Depending on the properties of the source, simulations predict an up to 9-fold reduction in pulse duration, whereas ≤50% of the peak intensity is maintained.

Laser-driven resonant magnetic soft-x-ray scattering for probing ultrafast antiferromagnetic and structural dynamics

Time-resolved resonant magnetic scattering in the soft-x-ray range is a powerful tool for accessing the spatially resolved and element-specific spin dynamics in magnetic materials. So far, the application of this photon-demanding technique was limited to large-scale facilities. However, upgrades to diffraction-limited storage rings supporting only x-ray pulses beyond 100 ps, and the shift of x-ray free-electron lasers toward attosecond pulses aggravate the competition for beamtime in the picosecond time window, which is of utmost relevance for magnetism research. Here we present the development of a lab-based instrument providing sufficient photon flux up to 1.5 keV photon energy covering the soft-x-ray resonances of transition and rare-earth metal atoms. Our setup features the mandatory tunability in energy and reciprocal space in combination with sub-10 ps temporal resolution, exploiting the broadband emission of a laser-driven plasma x-ray source, which is monochromatized to about 1 eV bandwidth by a reflection zone plate. We benchmark our approach against accelerator-based soft-x-ray sources by simultaneously probing the laser-induced magnetic and structural dynamics from an antiferromagnetically coupled Fe/Cr superlattice. Our development lays the foundation for laser-driven resonant scattering experiments to study ultrafast ordering phenomena of charges, spins, and orbitals.

Highly efficient soft x-ray spectrometer for transient absorption spectroscopy with broadband table-top high harmonic sources.

We present a novel soft x-ray spectrometer for ultrafast absorption spectroscopy utilizing table-top femtosecond high-order harmonic sources. Where most commercially available spectrometers rely on spherical variable line space gratings with a typical efficiency on the order of 3% in the first diffractive order, this spectrometer, based on a Hettrick–Underwood design, includes a reflective zone plate as a dispersive element. An improved efficiency of 12% at the N K-edge is achieved, accompanied by a resolving power of 890. The high performance of the soft x-ray spectrometer is further demonstrated by comparing nitrogen K-edge absorption spectra from calcium nitrate in aqueous solution obtained with our high-order harmonic source to previous measurements performed at the electron storage ring facility BESSY II.

Transient Sub-nanosecond Soft X-ray NEXAFS Spectroscopy on Organic Thin Films.

We demonstrate visible pump soft X-ray probe near-edge X-ray absorption fine structure (NEXAFS) spectroscopy measurements at the carbon K edge on thin molecular films in the laboratory. This opens new opportunities through the use of laboratory equipment for chemical speciation. We investigate the metal-free porphyrin derivative tetra(tert-butyl)porphyrazine as an ideal model system to elucidate electronic properties of tetrapyrroles like chlorophyll or heme. In contrast to measurements in gas or liquid state, the investigation of thin films is of high interest in the field of optoelectronic and photovoltaic devices though challenging due to the low damage thresholds of the samples upon excitation. With a careful pre-characterization using optical techniques, successful measurements were performed using a NEXAFS spectrometer based on a laser-produced plasma source and reflection zone plates with a resolving power of 1000 and a time resolution of 0.5 ns. In combination with density functional theory calculations, first insights into a long-lived excitonic state are gained and discussed.

Flat Field Soft X-ray Spectrometry with Reflection Zone Plates on a Curved Substrate

We report on the first experimental results obtained with a newly designed instrument for high-resolution soft X-ray spectroscopy, using reflection zone plates (RZPs) on a spherical substrate. The spectrometer was tested with a fluorescence source. High-resolution flat field spectra within ±50% around the design energies were measured at an interval of 150–750 eV, using only two RZPs: the first RZP, with its design energy of 277 eV, covered the band of 150–370 eV, and the second RZP, with a design energy of 459 eV, covered the band of 350–750 eV, where the upper boundary of this energy range was defined by the Ni coating of the RZPs. The absolute quantum efficiency of the spectrometer, including the optical element and the detector, was, on average, above 10%, and reached 20% at the designed energies of the RZPs. The resolving power E/∆E exceeded 600 for energies E inside the core range of 200–550 eV.

Holographic fiducial marks: A system for precise alignment of x-ray optics

This Letter covers the design and implementation of a generalizable system for the precise alignment of X-ray gratings. Next-generation high-energy grating-based Differential Phase Contrast (gDPC) X-ray imaging systems require precise alignment of the X-ray gratings as low as 1 mrad in rotation and 0.5 mm in translation. In this work, we designed holographic fiducial marks, consisting of four reflective Fresnel zone plates, each placed in a separate quadrant of the mark. When illuminated with a collimated laser beam, each mark creates a predefined pattern of four points, which changes quantitatively for any misalignment in each of the three translational and three rotational degrees of freedom. We fabricated the designed fiducial marks using photolithography and etching processes. The experimental system is implemented using a HeNe laser and an optical imaging system, which includes a beam expander, a plate beam splitter, and a CMOS camera, suitable for aligning practical gratings in gDPC X-ray imaging systems. Our experimental results demonstrate the rotational precision capabilities of the reported alignment system down to 0.42 mrad around the optical axis and 0.03 mrad around the axes perpendicular to the optical axis. The translational precision of 83.64 μm along the optical axis and 1.22 μm along the axes perpendicular to the optical axis is also demonstrated.

Towards Poisson noise limited optical pump soft X-ray probe NEXAFS spectroscopy using a laser-produced plasma source.

We present a laboratory setup for near edge X-ray absorption spectroscopy (NEXAFS) in the soft X-ray regime between 284 eV to 1303 eV with a resolving power of up to 1370. Based on a laser-produced plasma source, a pair of identical reflection zone plates and an X-ray CCD camera, the setup is intended for optical pump X-ray probe NEXAFS measurements with a detectable change in absorption of the excited sample down to 10-4 and 500 ps time resolution. Because of the high stability of the source the statistical error only depends on the detector response and the number of photons detected and can reach the detector noise limit after a couple of thousands single shots. Thus, structure-function relationship investigations of bio-molecules are rendered feasible in the laboratory.

X-ray spectroscopy with variable line spacing based on reflection zone plate optics.

X-ray spectroscopy is a method, ideally suited for investigating the electronic structure of matter, which has been enabled by the rapid developments in light sources and instruments. The x-ray fluorescence lines of life-relevant elements such as carbon, nitrogen, and oxygen are located in the soft x-ray regime and call for suitable spectrometer devices. In this Letter, we present a high-resolution spectrum of liquid water, recorded with a soft x-ray spectrometer based on a reflection zone plate (RZP) design. The RZP-based spectrometer with meridional variation of line space density from 2953 to 3757l/mm offers extremely high detection efficiency and, at the same time, medium energy resolution. We can reproduce the well-known splitting of liquid water in the lone pair regime with 10s acquisition time.

Note: Reflection zone plates as highly resolving broadband optics for soft X-ray laboratory spectrometers.

The resolving power and relative efficiency of two off-axis reflection zone plates (RZPs) in the soft X-ray range between 1 nm and 5 nm were investigated. RZPs focus only a very narrow bandwidth around the design wavelength. By misaligning the RZP, the focused wavelength can be tuned through a much wider spectral range. Using a laser-produced plasma source, we demonstrate that a single RZP can be efficiently used for spectroscopy at arbitrary wavelengths in the investigated soft X-ray range.

Polycapillary-boosted instrument performance in the extreme ultraviolet regime for inverse photoemission spectroscopy.

A collimating polycapillary half lens, traditionally used in the medium and hard X-ray band, is operated at a photon energy of 36 eV for the first time. While the transmission still exceeds 50%, the measured and simulated spatial resolution and angular divergence approach 0.4 mm or less and at most 20 mrad, respectively. This unexpected, superior performance of the polycapillary optic in the extreme Ultraviolet could enable the design of an efficient, versatile and compact spectrometer for inverse photoemission spectroscopy (IPES): Its wavelength-dispersive component, a customized reflection zone plate, can maintain an energy resolution of 0.3 eV, whereas the sensitivity may be enhanced by more than one order of magnitude, compared to conventional spectrometers. Furthermore, the overall length of 0.9 m would allow for an eased alignment and evacuation. We see a significant potential for numerous polycapillary-based XUV / soft X-ray instruments in the future, in particular after further optimization for this long wavelength regime.

Highly efficient soft X-ray spectrometer based on a reflection zone plate for resonant inelastic X-ray scattering measurements.

We present a newly designed compact and flexible soft X-ray spectrometer for resonant inelastic X-ray scattering (RIXS) studies within an energy range from 380 eV to 410 eV, which would include the K alpha emission lines of vital elements like nitrogen. We utilized an off-axis reflection zone plate (RZP) as the wavelength selective element with a maximum line density of 10000 l/mm. A higher energy resolution over a broader range of ± 15 eV around the designed energy was achieved by displacing the RZP. Additionally, for the first time, an actual optical side effect, the so-called comatic aberration was exploited to increase the energy resolution. First results show a resolving power in the order of 1300 for photon energy of 395 eV, which is comparable to a commercial varied line spacing grating (VLS).

Reflection zone plate concept for resonant inelastic x-ray scattering spectrometry.

We simulate a proof-of-principle design of a wavelength dispersive, parallel spectrometer for use in resonant inelastic x-ray scattering (RIXS). The instrument relies on a multiple-channel reflection zone plate (RZP) array, enabling the recording of fluorescence spectra from an acceptance angle of 18 arc min×19 arc min with a mainly source-size-limited resolving power of (0.2-2.6)×104 over an energy range of 21 eV at the L-edge of Fe around 715 eV. An optimal two-dimensional signal readout preserves the spectral resolution to a large extent for widely open exit apertures of ≳50 mm2. The geometrical parameters are matched to the PEAXIS end station at the BESSY II synchrotron facility, and relaxed RZP line densities of <9×102 mm-1 assure the technical feasibility. An error budget estimation with respect to fabrication and alignment tolerances provides the link to real, RZP-based RIXS experiments in the future.

A desktop extreme ultraviolet microscope based on a compact laser-plasma light source

A compact, desktop size microscope, based on laser-plasma source and equipped with reflective condenser and diffractive Fresnel zone plate objective, operating in the extreme ultraviolet (EUV) region at the wavelength of 13.8 nm, was developed. The microscope is capable of capturing magnified images of objects with 95-nm full-pitch spatial resolution (48 nm 25–75% KE) and exposure time as low as a few seconds, combining reasonable acquisition conditions with stand-alone desktop footprint. Such EUV microscope can be regarded as a complementary imaging tool to already existing, well-established ones. Details about the microscope, characterization, resolution estimation and real sample images are presented and discussed.

Single shot near edge x-ray absorption fine structure spectroscopy in the laboratory

With the help of adapted off-axis reflection zone plates, near edge X-ray absorption fine structure spectra at the C and N K-absorption edge have been recorded using a single 1.2 ns long soft X-ray pulse. The transmission experiments were performed with a laser-produced plasma source in the laboratory rendering time resolved measurements feasible independent on large scale facilities. A resolving power of E/ΔE ∼ 950 at the respective edges could be demonstrated. A comparison of single shot spectra with those collected with longer measuring time proves that all features of the used reference samples (silicon nitrate and polyimide) can be resolved in 1.2 ns. Hence, investigations of radiation sensitive biological specimen become possible due to the high efficiency of the optical elements enabling low dose experiments.

The At-Wavelength Metrology Facility at BESSY-II

The At-Wavelength Metrology Facility at BESSY-II is dedicated to short-term characterization of novel UV, EUV and XUV optical elements, such as diffraction gratings, mirrors, multilayers and nano-optical devices like reflection zone plates. It consists of an Optics Beamline PM-1 and a Reflectometer in a clean-room hutch as a fixed end station. The bending magnet Beamline is a Plane Grating Monochromator beamline (c-PGM) equipped with an SX700 monochromator. The beamline is specially tailored for efficient high-order suppression and stray light reduction. The versatile 11-axes UHV-Reflectometer can house life-sized optical elements, which are fully adjustable and of which the reflection properties can be measured in the full incidence angular range as well as in the full azimuthal angular range to determine polarization properties.