Synchrotron Beamlines Research Articles

Fifteen Years of Radionuclide Research at the KIT Synchrotron Source in the Context of the Nuclear Waste Disposal Safety Case

For more than 120 years, systematic studies of X-ray interaction with matter have been the basis for our understanding of materials—both of natural or man-made origin—and their structure-function relationships. Beginning with simple radiographic imaging at the end of the 19th century, X-ray based analytical tools such as X-ray diffraction, X-ray fluorescence and photoemission or X-ray absorption techniques are indispensable in almost any field of chemical and material sciences—including basic and applied actinide and radionuclide studies. The advent of dedicated synchrotron radiation (SR) sources in the second half of the last century has revolutionized the analytical power of X-ray probes, while—with increasing number of SR facilities—beamline instrumentation followed a trend towards increasing specialization and adaption to a major research topic. The INE-Beamline and ACT station at the KIT synchrotron source belong to the exclusive club of a few synchrotron beamline facilities—mostly located in Europe—dedicated to the investigation of highly radioactive materials. Since commissioning of the INE-Beamline in 2005, capabilities for synchrotron-based radionuclide and actinide sciences at KIT have been continuously expanded, driven by in-house research programs and external user needs.

Development of Synchrotron Footprinting at NSLS and NSLS-II.

First developed in the 1990's at the National Synchrotron Light Source, xray synchrotron footprinting is an ideal technique for the analysis of solution-state structure and dynamics of macromolecules. Hydroxyl radicals generated in aqueous samples by intense x-ray beams serve as fine probes of solvent accessibility, rapidly and irreversibly reacting with solvent exposed residues to provide a "snapshot" of the sample state at the time of exposure. Over the last few decades, improvements in instrumentation to expand the technology have continuously pushed the boundaries of biological systems that can be studied using the technique. Dedicated synchrotron beamlines provide important resources for examining fundamental biological mechanisms of folding, ligand binding, catalysis, transcription, translation, and macromolecular assembly. The legacy of synchrotron footprinting at NSLS has led to significant improvement in our understanding of many biological systems, from identifying key structural components in enzymes and transporters to in vivo studies of ribosome assembly. This work continues at the XFP (17-BM) beamline at NSLS-II and facilities at ALS, which are currently accepting proposals for use.

Far-infrared self-continuum absorption of H216O and H218O (15–500 cm−1)

The water vapor continuum absorption is studied in a spectral range covering most of the pure rotational spectrum of water molecule up to 500 cm−1. The continuum absorption was derived from the broadband water vapor spectra recorded by Fourier transform spectrometer equipped with the 151-m multipass gas cell at the AILES beam line of the SOLEIL synchrotron. The coherent (10–35 cm−1) and standard (40–500 cm−1) radiation modes of the synchrotron were used. In order to refine the magnitude and clarify the physical origin of the continuum, spectra of the two major water isotopologues, H216O and H218O, were considered. Recordings at several water vapor pressures were used to check the expected quadratic pressure dependence of the continuum.The new data extend and supplement previous measurements filling, in particular, the gap between 200 and 350 cm−1, which was never studied before. The H216O and H218O absorption continua in the range of 50–650 cm−1 show similar frequency dependence and magnitude. In particular, both continua exhibit a clear water dimer spectral signature near 15 cm−1, in good agreement with previous ab initio calculations. The present data confirm that the MT-CKD empirical continuum model widely used in atmospheric applications, overestimates importantly the continuum magnitude in the whole range of the rotational band. The observed irregular frequency dependence of the retrieved self-continuum cross-section values is tentatively interpreted as due to uncertainties on the resonance lines of the water monomer spectrum which is subtracted from the recorded spectra. On the basis of spectra simulations, the inadequate description of the line shapes in the range of the intermediate wings (detuning of 5–10 cm−1 from line center) and the uncertainties on the self-broadening coefficients of water monomer lines are identified as possible mechanisms responsible of the observed irregular fluctuations.

Surface shape determination with a stitching Michelson interferometer and accuracy evaluation.

Stitching methods are increasingly used for determining the surface shape of large and high precision optical elements used in synchrotron beamlines. They consist in reconstructing the surface topography from multiple measurements on overlapping parts of the optics aperture by various algorithms. This paper is an attempt to investigate how true and accurate such a reconstruction can be. Error sources are identified and evaluated throughout the acquisition and processing steps. The analysis is based on the example SOLEIL Michelson interferometer for nano-topography, a dedicated measurement bench for stitching interferometry. We propose a method for determining the error made on the estimate of the interferometric reference surface from the stitching dataset. This determination is made before and independently of the stitching procedure itself.

Grating metrology for X-ray and V-UV synchrotron beamlines at SOLEIL.

Diffraction gratings are key elements of soft X-ray synchrotron beamlines. Besides wavelength dispersion, specific parameters can be tailored to adjust the energy dependent efficiency and focusing, and to correct wavefront aberrations. As key elements of a beamline, any departure from the design values can severely reduce the overall performance. On the other hand, known non-conformities can often be corrected by slight adjustment of the alignment parameters. A careful and accurate metrology is therefore required before installation on the beamline. After presenting what variable line spacing gratings, variable groove depth gratings, and alternate multilayer gratings are, the use of the SOLEIL long trace profiler for the measurement of groove density variation along the surface and of the atomic force microscope for the groove geometry and roughness characterizations will be discussed. A few examples of grating metrology will be presented and analyzed with the help of optical simulations.

Stitching techniques for measuring X-ray synchrotron mirror topography.

Optical metrology and polishing techniques are continuously evolving to satisfy the increasingly stringent specifications required for X-ray optical components for synchrotron and free-electron laser light source beamlines. For both spherical and aspherical geometries, the most demanding applications may have target residual figure errors close to 1 nm. To achieve such specifications and maintain them in the optomechanical mount, it is critical to develop methods capable of measuring the topography of the optical surface over the clear aperture of the mirror. The European Synchrotron Radiation Facility optical metrology laboratory has developed a stitching tool initially aimed at measuring long flat mirrors up to 1 m long with a Fizeau interferometer. The system is routinely used providing 2D maps of the optical surface. The instrument capabilities have been extended to characterize moderately curved optics using a transmission flat element, and results obtained on a high quality spherical mirror with 120 m of radius of curvature are presented. As a novel approach of stitching application, the technique has been used to improve the measurement accuracy of the Fizeau interferometer when measuring short plane mirrors. Acquisition of 2D topographies on a short plane mirror by micro-stitching interferometry is also presented and discussed.

Conceptual Design for a Microfocus Beamline on the SKIF Synchrotron

A design is proposed for a fourth-generation synchrotron beamline for investigating the structure and composition of a broad range of samples with high (submicron) spatial resolution.

A methodology study on chemical and molecular structure imaging in modified forage leaf tissue with cutting-edge synchrotron-powered technology (SR-IMS) as a potential research tool.

To date there is no any study on imaging molecular chemistry and chemical structure of biotech-modified plant tissue on a molecular basis. The objective of this methodology study was to apply a non-invasive and non-destructive synchrotron powered technology - SR-IMS to image molecular chemistry of the modified forage leaf tissue. The infrared molecular vibrational microspectroscopy powered with synchrotron light at Advanced Light Source (ALS, Lawrence Berkeley National Lab, Berkeley, California, Dept. of Energy, USA) were applied. The synchrotron beamline time was arranged by National Synchrotron Light Source (Scientist Dr. Lisa Miller, Brookhaven National Lab, Dept. of Energy, USA). The various molecular functional groups in the forage tissue included CH symmetric and asymmetric regions, amides I and II regions, structure and non-structure CHO regions, carbonyl ester region with peak areas at ca. 3644-3000 cm-1, ca 3005-2979 cm-1, ca. 1722-1483 cm-1, ca. 1488-1412 cm-1, ca. 1296-1189 cm-1, and ca. 1194-951 cm-1. The spectral peak area ratio imaging of chemical functional groups were also studied which included the ratio of peak area under ca. 1722-1483 cm-1 to peak area under ca. 3005-2979 cm-1 and the ratio of peak area under ca. 1722-1483 cm-1 to peak area under ca. 1194-951 cm-1. The results showed that the advanced synchrotron-based technology - SR-IMS was able to image the forage tissue at an ultra-highly resolution within intact tissue within cellular and subcellular dimension. It revealed the forage tissue in a molecular chemical sense and provided an insight on nutrient properties and their molecular structure as well as chemical features. In conclusion, the synchrotron-radiation SR-IMS is able to image molecular structure of the forage leaf tissue at an ultra-highly resolution. The advanced SR-IMS technique could provide leaf tissue four kinds of information simultaneously: tissue structure, tissue chemistry, tissue nutrients, and tissue environment of forage.

Nanoporous gold: a hierarchical and multiscale 3D test pattern for characterizing X-ray nano-tomography systems.

Full-field transmission X-ray microscopy (TXM) is a well established technique, available at various synchrotron beamlines around the world as well as by laboratory benchtop devices. One of the major TXM challenges, due to its nanometre-scale resolution, is the overall instrument stability during the acquisition of the series of tomographic projections. The ability to correct for vertical and horizontal distortions of each projection image during acquisition is necessary in order to achieve the effective 3D spatial resolution. The effectiveness of such an image alignment is also heavily influenced by the absorption properties and strong contrast of specific features in the scanned sample. Here it is shown that nanoporous gold (NPG) can be used as an ideal 3D test pattern for evaluating and optimizing the performance of a TXM instrument for hard X-rays at a synchrotron beamline. Unique features of NPG, such as hierarchical structures at multiple length scales and high absorbing capabilities, makes it an ideal choice for characterization, which involves a combination of a rapid-alignment algorithm applied on the acquired projections followed by the extraction of a set of both 2D- and 3D-descriptive image parameters. This protocol can be used for comparing the efficiency of TXM instruments at different synchrotron beamlines in the world or benchtop devices, based on a reference library of scanned NPG samples, containing information about the estimated horizontal and vertical alignment values, 2D qualitative parameters and quantitative 3D parameters. The possibility to tailor the ligament sizes of NPG to match the achievable resolution in combination with the high electron density of gold makes NPG an ideal 3D test pattern for evaluating the status and performance of a given synchrotron-based or benchtop-based TXM setup.

Influence of source size and spectral bandwidth on the imaging of a zone plate

Direct X-ray imaging by a Fresnel zone plate (FZP) has achieved a spatial resolution of 10 nm on a synchrotron beamline. It may be used to obtain submicron-resolution X-ray images of laser-plasma sources or fusion targets. However, none of previous imaging experiments with laser-plasma kilo-elelctron-volt X-ray sources shows such a high resolution. In comparison with the FZP imaging on a synchrotron, we consider a case of imaging an extended object with a laser-plasma X-ray source that the illumination monochromaticity is lower and the field of view larger. Our simulations show that the spatial resolution is affected by both the object size and the spectral bandwidth of the source, which can explain the previous experiments. We conclude that by using a 100-zone FZP to image an object with up to 700 μm in size, a spatial resolution better than 1 μm can be realized by using X-rays of several kilo-electron volts and a spectral bandwidth just less than 3%. In this paper, we report a proof-of-principle study in simulation and experiment in an optical range centered at 632.8 nm. The simulation is performed with the same method as that previously used for X-ray imaging but with a 100-zone FZP working in the optical range. Simulations show that with the increase of the object size, the field-of-view contrast is degraded, but the spatial resolution is nearly unchanged. With the increase of the spectral bandwidth for the illumination, both the contrast and the resolution are degraded. In the experiments, different spectral bandwidths are realized by band-pass filters and different object sizes by an adjustable aperture. The experimental results are confirmed to be in agreement with the simulations. These results reveal that given a satisfied spectral bandwidth of laser-plasma X rays, the FZP imaging will be a promising approach to 1 μm or higher resolution X-ray imaging of a 1-mm-size object.

Dynamic adaptive X-ray optics. Part I. Time-resolved optical metrology investigation of the bending behaviour of piezoelectric bimorph deformable X-ray mirrors.

Piezoelectric bimorph deformable mirrors (`bimorphs') are routinely used on many synchrotron and free-electron laser beamlines to provide active variation in the size and shape of the X-ray beam. However, the time-domain potential of such optics has never been fully exploited. For the first time, the fast dynamic bending response of bimorphs is investigated here using Fizeau interferometry. Automated scripts for acquisition and analysis were developed to collect Fizeau data at a rate of 0.1 Hz to record dynamic changes in the optical surface as voltages were applied to the electrodes of the piezoelectric actuators. It is demonstrated that residual drift in the tangential radius of curvature of a bimorph can be significantly reduced using enhanced opto-mechanical holders and a fast programmable high-voltage power supply. Further improvements are achieved by applying small opposing voltages to compensate for piezoelectric creep. The present study shows that bimorphs can truly be used as high-speed adaptive optics for the X-ray domain, even without closed-loop feedback correction. This opens the possibility for relatively simple real-time tuning of the profile of X-ray bimorphs. Part II of this study [Alcock, Nistea, Signorato, Owen, Axford, Sutter, Foster & Sawhney (2019), J. Synchrotron Rad. 26, 45-51] builds upon these results and demonstrates how bimorphs can rapidly provide customisable sizes and shapes of synchrotron X-ray beams, specifically tailored to suit the experimental samples being investigated.

Dynamic adaptive X-ray optics. Part II. High-speed piezoelectric bimorph deformable Kirkpatrick-Baez mirrors for rapid variation of the 2D size and shape of X-ray beams.

The tangential curvature of actively bent X-ray mirrors at synchrotron radiation and X-ray free-electron laser (XFEL) facilities is typically only changed every few hours or even days. This operation can take tens of minutes for active optics with multiple bending actuators and often requires expert guidance using in situ monitoring devices. Hence, the dynamic performance of active X-ray optics for synchrotron beamlines has historically not been exploited. This is in stark contrast to many other scientific fields. However, many areas of synchrotron radiation and XFEL science, including macromolecular crystallography, could greatly benefit from the ability to change the size and shape of the X-ray beam rapidly and continuously. The advantages of this innovative approach are twofold: a large reduction in the dead time required to change the size of the X-ray beam for different-sized samples and the possibility of making multiple changes to the beam during the measurement of a single sample. In the preceding paper [Part I; Alcock, Nistea, Signorato & Sawhney (2019), J.Synchrotron Rad. 26, 36-44], which accompanies this article, high-speed visible-light Fizeau interferometry was used to identify the factors which influence the dynamic bending behaviour of piezoelectric bimorph deformable X-ray mirrors. Building upon this ex situ metrology study, provided here is the first synchrotron radiation beamline implementation of high-speed adaptive X-ray optics using two bimorphs operating as a Kirkpatrick-Baez pair. With optimized substrates, novel opto-mechanical holders and a next-generation high-voltage power supply, the size of an X-ray beam was rapidly and repeatedly switched in <10 s. Of equal importance, it is also shown that compensation of piezoelectric creep ensures that the X-ray beam size remains stable for more than 1 h after making a major change. The era of high-speed adaptive X-ray optics for synchrotron radiation and XFEL beamlines has begun.

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.

A versatile shear cell for investigation of structure of food materials under shear

A versatile cell for X-ray and neutron scattering experiments on samples under shear has been designed. To our knowledge, it is the first shear cell which can be used for both SAXS and SANS in respectively synchrotron or reactor beamlines. The cell is mainly intended for scattering experiments in so-called “1–2 plane geometry”, but can also be modified into cone–plate and plate–plate rheological geometries, giving access to the 1–3 scattering plane. The latter two geometries, however, can only be used with neutron scattering. The final cell design is compact, which allows it to be used even with lab-based X-ray sources. A special thermostatic shell allows for the temperature control of the samples under investigation in the range from 5 up to 100 °C. Several X-ray and neutron scattering experiments performed with the cell have helped in better understanding of the structuring under shear of food materials, such as: cellulose suspensions, fat crystal networks and milk proteins.

Real-Time Investigation of Recovery, Recrystallization and Austenite Transformation during Annealing of a Cold-Rolled Steel Using High Energy X-ray Diffraction (HEXRD)

The annealing process of cold-rolled ferrite/pearlite steel involves numerous metallurgical mechanisms as recovery/recrystallization of deformed phases, ripening of carbide microstructure, and austenite transformation in the intercritical domain. The interactions between these mechanisms govern the morphogenesis of the transformed austenite microstructure and, thus, the final properties of the steel. This paper demonstrates that high energy X-ray diffraction (HEXRD) on synchrotron beamline offers the unique possibility to follow concomitantly these mechanisms in situ during a single experiment. A cold-rolled ferrite-pearlite steel dedicated to the industrial production of Dual-Phase steel serves as case-study. Synchrotron experiments have been conducted in transmission at 100 keV with a 2D detector. Diffraction patterns acquired all along an annealing treatment are first analyzed after circular integration. A Rietveld refinement procedure coupled with a Williamson-Hall approach is used to determine phase transformation and recovery kinetics. In this paper, a new method inspired by the 3D X-ray diffraction tomography is proposed to follow recrystallization kinetics at the same time. It is based on a systematic detection of individual diffraction spots related to newly recrystallized grains appearing on Debye-Scherrer rings. The deduced recrystallization kinetics is compared and validated by more conventional ex situ methods.

Size-exclusion chromatography small-angle X-ray scattering of water soluble proteins on a laboratory instrument.

Coupling of size-exclusion chromatography with biological solution small-angle X-ray scattering (SEC-SAXS) on dedicated synchrotron beamlines enables structural analysis of challenging samples such as labile proteins and low-affinity complexes. For this reason, the approach has gained increased popularity during the past decade. Transportation of perishable samples to synchrotrons might, however, compromise the experiments, and the limited availability of synchrotron beamtime renders iterative sample optimization tedious and lengthy. Here, the successful setup of laboratory-based SEC-SAXS is described in a proof-of-concept study. It is demonstrated that sufficient quality data can be obtained on a laboratory instrument with small sample consumption, comparable to typical synchrotron SEC-SAXS demands. UV/vis measurements directly on the SAXS exposure cell ensure accurate concentration determination, crucial for direct molecular weight determination from the scattering data. The absence of radiation damage implies that the sample can be fractionated and subjected to complementary analysis available at the home institution after SEC-SAXS. Laboratory-based SEC-SAXS opens the field for analysis of biological samples at the home institution, thus increasing productivity of biostructural research. It may further ensure that synchrotron beamtime is used primarily for the most suitable and optimized samples.

Enabling liquid vapor analysis using synchrotron VUV single photon ionization mass spectrometry with a microfluidic interface.

Vacuum ultraviolet (VUV) single photon ionization mass spectrometry (SPI-MS) is a vacuum-based technique typically used for the analysis of gas phase and solid samples, but not for liquids due to the challenge in introducing volatile liquids in a vacuum. Here we present the first demonstration of in situ liquid analysis by integrating the System for Analysis at the Liquid Vacuum Interface (SALVI) microfluidic reactor into VUV SPI-MS. Four representative volatile organic compound (VOC) solutions were used to illustrate the feasibility of liquid analysis. Our results show the accurate mass identification of the VOC molecules and the reliable determination of appearance energy that is consistent with ionization energy for gaseous species in the literature as reported. This work validates that the vacuum-compatible SALVI microfluidic interface can be utilized at the synchrotron beamline and enable the in situ study of gas-phase molecules evaporating off the surface of a liquid, which holds importance in the study of condensed matter chemistry.

Towards chemically neutral carbon cleaning processes: plasma cleaning of Ni, Rh and Al reflective optical coatings and thin Al filters for free-electron lasers and synchrotron beamline applications

The choice of a reflective optical coating or filter material has to be adapted to the intended field of application. This is mainly determined by the required photon energy range or by the required reflection angle. Among various materials, nickel and rhodium are common materials used as reflective coatings for (soft) X-ray mirrors. Similarly, aluminium is one of the most commonly used materials for extreme ultraviolet and soft X-ray transmission filters. However, both of these types of optics are subject to carbon contamination, which can be increasingly problematic for the operation of the high-performance free-electron laser and synchrotron beamlines. As an attempt to remove this type of contamination, an inductively coupled plasma source has been used in conjunction with N2/O2/H2 and N2/H2 feedstock gas plasmas. Results from the chemical surface analysis of the above materials before and after plasma treatment using X-ray photoelectron spectroscopy are reported. It is concluded that a favorable combination of an N2/H2 plasma feedstock gas mixture leads to the best chemical surface preservation of Ni, Rh and Al while removing the carbon contamination. However, this feedstock gas mixture does not remove C contamination as rapidly as, for example, an N2/O2/H2 plasma which induces the surface formation of NiO and NiOOH in Ni and RhOOH in Rh foils. As an applied case, the successful carbon removal from ultrathin Al filters previously used at the FERMI FEL1 using an N2/H2 plasma is demonstrated.

Synthesis of FeN4 at 180 GPa and its crystal structure from a submicron-sized grain.

Iron tetra-nitride, FeN4, was synthesized from the elements in a laser-heated diamond anvil cell at 180 (5) GPa and 2700 (200) K. Its crystal structure was determined based on single-crystal X-ray diffraction data collected from a submicron-sized grain at the synchrotron beamline ID11 of ESRF. The compound crystallizes in the triclinic space group P . In the asymmetric unit, the Fe atom occupies an inversion centre (Wyckoff position 1d), while two N atoms occupy general positions (2i). The structure is made up from edge-sharing [FeN6] octa-hedra forming chains along [100] and being inter-connected through N-N bridges. N atoms form catena-poly[tetraz-1-ene-1,4-di-yl] anions [-N=N-N-N-]∞ 2- running along [001]. In comparison with the previously reported structure of FeN4 at 135 GPa [Bykov et al. (2018). Nat. Commun. 9, 2756], the crystal structure of FeN4 at 180 GPa is similar but the structural model is significantly improved in terms of the precision of the bond lengths and angles.

Tomosaic: efficient acquisition and reconstruction of teravoxel tomography data using limited-size synchrotron X-ray beams.

X-rays offer high penetration with the potential for tomography of centimetre-sized specimens, but synchrotron beamlines often provide illumination that is only millimetres wide. Here an approach is demonstrated termed Tomosaic for tomographic imaging of large samples that extend beyond the illumination field of view of an X-ray imaging system. This includes software modules for image stitching and calibration, while making use of existing modules available in other packages for alignment and reconstruction. The approach is compatible with conventional beamline hardware, while providing a dose-efficient method of data acquisition. By using parallelization on a distributed computing system, it provides a solution for handling teravoxel-sized or larger datasets that cannot be processed on a single workstation in a reasonable time. Using experimental data, the package is shown to provide good quality three-dimensional reconstruction for centimetre-sized samples with sub-micrometre pixel size.