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Two‐directional beam‐tracking (2DBT) is a method for phase‐contrast imaging and tomography that uses an intensity modulator to structure the X‐ray beam into an array of independent circular beamlets that are resolved by a high‐resolution detector. It features isotropic spatial resolution, provides two‐dimensional phase sensitivity, and enables the three‐dimensional reconstructions of the refractive index decrement, δ, and the attenuation coefficient, μ. In this work, the angular sensitivity and the spatial resolution of 2DBT images in a synchrotron‐based implementation is reported. In its best configuration, angular sensitivities of ∼20 nrad and spatial resolution of at least 6.25 µm in phase‐contrast images were obtained. Exemplar application to the three‐dimensional imaging of soft tissue samples, including a mouse liver and a decellularized porcine dermis, is also demonstrated. [ABSTRACT FROM AUTHOR]

X-ray dark-field or ultra-small angle scatter imaging has become increasingly important since the introduction of phase-based x-ray imaging and is having transformative impact in fields such as in vivo lung imaging and explosives detection. Here, we show that dark-field images acquired with the edge-illumination method (either in its traditional double mask or simplified single mask implementation) provide a direct measurement of the scattering function, which is unaffected by system-specific parameters such as the autocorrelation length. We show that this is a consequence both of the specific measurement setup and of the mathematical approach followed to retrieve the dark-field images. We show agreement with theoretical models for datasets acquired both with synchrotron and laboratory x-ray sources. We also introduce a new contrast mechanism, the variance of refraction, which is extracted from the same dataset and provides a direct link with the size of the scattering centers. We show that this can also be described by the same theoretical models. We study the behavior of both signals vs key parameters such as x-ray energy and scatterer radius. We find this allows quantitative and direct scattering measurements during imaging, with implications in all fields where dark-field imaging is used. [ABSTRACT FROM AUTHOR]

Background: Microscopic imaging of cartilage is a key tool for the study and development of treatments for osteoarthritis. When cellular and sub‐cellular resolution is required, histology remains the gold standard approach, albeit limited by the lack of volumetric information as well as by processing artifacts. Cartilage imaging with the sub‐cellular resolution has only been demonstrated in the synchrotron environment. Purpose: To provide a proof‐of‐concept demonstration of the capability of a laboratory‐based x‐ray phase‐contrast microscope to resolve sub‐cellular features in a cartilage sample. Methods: This work is based on a laboratory‐based x‐ray microscope using intensity‐modulation masks. The structured nature of the beam, resulting from the mask apertures, allows the retrieval of three contrast channels, namely, transmission, refraction and dark‐field, with resolution depending only on the mask aperture width. An ex vivo equine cartilage sample was imaged with the x‐ray microscope and results were validated with synchrotron tomography and histology. Results: Individual chondrocytes, that is, cells responsible for cartilage formation, could be detected with the laboratory‐based microscope. The complementarity of the three retrieved contrast channels allowed the detection of sub‐cellular features in the chondrocytes. Conclusions: We provide the first proof‐of‐concept of imaging cartilage tissue with sub‐cellular resolution using a laboratory‐based x‐ray microscope. [ABSTRACT FROM AUTHOR]

Diffractive optical elements such as periodic gratings are fundamental devices in X‐ray imaging – a technique that medical, material science, and security scans rely upon. Fabrication of such structures with high aspect ratios at the nanoscale creates opportunities to further advance such applications, especially in terms of relaxing X‐ray source coherence requirements. This is because typical grating‐based X‐ray phase imaging techniques (e.g., Talbot self‐imaging) require a coherence length of at least one grating period and ideally longer. In this paper, the fabrication challenges in achieving high‐aspect ratio nanogratings filled with gold are addressed by a combination of laser interference and nanoimprint lithography, physical vapor deposition, metal assisted chemical etching (MACE), and electroplating. This relatively simple and cost‐efficient approach is unlocked by an innovative post‐MACE drying step with hexamethyldisilazane, which effectively minimizes the stiction of the nanostructures. The theoretical limits of the approach are discussed and, experimentally, X‐ray nanogratings with aspect ratios >40 are demonstrated. Finally, their excellent diffractive abilities are shown when exposed to a hard (12.2 keV) monochromatic X‐ray beam at a synchrotron facility, and thus potential applicability in phase‐based X‐ray imaging. [ABSTRACT FROM AUTHOR]

The advent of hard X-ray free-electron lasers enables nanoscopic X-ray imaging with sub-picosecond temporal resolution. X-ray grating interferometry offers a phase-sensitive full-field imaging technique where the phase retrieval can be carried out from a single exposure alone. Thus, the method is attractive for imaging applications at X-ray free-electron lasers where intrinsic pulse-to-pulse fluctuations pose a major challenge. In this work, the single-exposure phase imaging capabilities of grating interferometry are characterized by an implementation at the I13-1 beamline of Diamond Light Source (Oxfordshire, UK). For comparison purposes, propagation-based phase contrast imaging was also performed at the same instrument. The characterization is carried out in terms of the quantitativeness and the contrast-to-noise ratio of the phase reconstructions as well as via the achievable spatial resolution. By using a statistical image reconstruction scheme, previous limitations of grating interferometry regarding the spatial resolution can be mitigated as well as the experimental applicability of the technique. [ABSTRACT FROM AUTHOR]

Full‐field transmission X‐ray microscopy (TXM) is a very potent high‐resolution X‐ray imaging technique. However, it is challenging to achieve fast acquisitions because of the limited efficiency of the optics. Using a broader energy bandwidth, for example using a multilayer monochromator, directly increases the flux in the experiment. The advantage of more counts needs to be weighed against a deterioration in achievable resolution because focusing optics show chromatic aberrations. This study presents theoretical considerations of how much the resolution is affected by an increase in bandwidth as well as measurements at different energy bandwidths (ΔE/E = 0.013%, 0.27%, 0.63%) and the impact on achievable resolution. It is shown that using a multilayer monochromator instead of a classical silicon double‐crystal monochromator can increase the flux by an order of magnitude with only a limited effect on the resolution. [ABSTRACT FROM AUTHOR]

X‐ray ptychography and X‐ray fluorescence are complementary nanoscale imaging techniques, providing structural and elemental information, respectively. Both methods acquire data by scanning a localized beam across the sample. X‐ray ptychography processes the transmission signal of a coherent illumination interacting with the sample, to produce images with a resolution finer than the illumination spot and step size. By enlarging both the spot and the step size, the technique can cover extended regions efficiently. X‐ray fluorescence records the emitted spectra as the sample is scanned through the localized beam and its spatial resolution is limited by the spot and step size. The requisites for fast ptychography and high‐resolution fluorescence appear incompatible. Here, a novel scheme that mitigates the difference in requirements is proposed. The method makes use of two probes of different sizes at the sample, generated by using two different energies for the probes and chromatic focusing optics. The different probe sizes allow to reduce the number of acquisition steps for the joint fluorescence–ptychography scan compared with a standard single beam scan, while imaging the same field of view. The new method is demonstrated experimentally using two undulator harmonics, a Fresnel zone plate and an energy discriminating photon counting detector. [ABSTRACT FROM AUTHOR]

Understanding catalyst deactivation by coking is crucial for knowledge‐based catalyst and process design in reactions with carbonaceous species. Post‐mortem analysis of catalyst coking is often performed by bulk characterization methods. Here, hard X‐ray ptychographic computed tomography (PXCT) was used to study Ni/Al2O3 catalysts for CO2 methanation and CH4 dry reforming after artificial coking treatment. PXCT generated quantitative 3D maps of local electron density at ca. 80 nm resolution, allowing to visualize and evaluate the severity of coking in entire catalyst particles of ca. 40 μm diameter. Coking was primarily revealed in the nanoporous solid, which was not detectable in resolved macropores. Coke formation was independently confirmed by operando Raman spectroscopy. PXCT is highlighted as an emerging characterization tool for nanoscale identification, co‐localization, and potentially quantification of deactivation phenomena in 3D space within entire catalyst particles. [ABSTRACT FROM AUTHOR]

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For imaging events of extremely short duration, like shock waves or explosions, it is necessary to be able to image the object with a single-shot exposure. A suitable setup is given by a laser-induced X-ray source such as the one that can be found at GSI (Helmholtzzentrum für Schwerionenforschung GmbH) in Darmstadt (Society for Heavy Ion Research), Germany. There, it is possible to direct a pulse from the high-energy laser Petawatt High Energy Laser for Heavy Ion eXperiments (PHELIX) on a tungsten wire to generate a picosecond polychromatic X-ray pulse, called backlighter. For grating-based single-shot phase-contrast imaging of shock waves or exploding wires, it is important to know the weighted mean energy of the X-ray spectrum for choosing a suitable setup. In propagation-based phase-contrast imaging the knowledge of the weighted mean energy is necessary to be able to reconstruct quantitative phase images of unknown objects. Hence, we developed a method to evaluate the weighted mean energy of the X-ray backlighter spectrum using propagation-based phase-contrast images. In a first step wave-field simulations are performed to verify the results. Furthermore, our evaluation is cross-checked with monochromatic synchrotron measurements with known energy at Diamond Light Source (DLS, Didcot, UK) for proof of concepts. [ABSTRACT FROM AUTHOR]

We present here a new method of performing X-ray edge-subtraction ptychographic imaging by combining multiple harmonics from an undulator synchtrotron source and an energy discriminating photon counting detector. Conventionally, monochromatic far-field X-ray ptychography is used to perform edge subtraction through the use of multiple monochromatic energy scans to obtain spectral information for a variety of applications. Here, we use directly the undulator spectrum from a synchrotron source, selecting two separate harmonics post sample using the Pixirad-1/Pixie-III detector. The result is two monochromatic images, above and below an absorption edge of interest. The proposed method is applied to obtain Au L-edge subtraction imaging of a Au-Ni grid test sample. The Au L-edge subtraction is particularly relevant for the identification of gold nanoparticles for biomedical applications. Switching the energy scan mechanism from a mechanical monochromator to an electronic detector threshold allows for faster spectral data collection with improved stability. [ABSTRACT FROM AUTHOR]

Multilayer monochromator devices are commonly used at (imaging) beamlines of synchrotron facilities to shape the X‐ray beam to relatively small bandwidth and high intensity. However, stripe artefacts are often observed and can deteriorate the image quality. Although the intensity distribution of these artefacts has been described in the literature, their spectral distribution is currently unknown. To assess the spatio‐spectral properties of the monochromated X‐ray beam, the direct beam has been measured for the first time using a hyperspectral X‐ray detector. The results show a large number of spectral features with different spatial distributions for a [Ru, B4C] strip monochromator, associated primarily with the higher‐order harmonics of the undulator and monochromator. It is found that their relative contributions are sufficiently low to avoid an influence on the imaging data. The [V, B4C] strip suppresses these high‐order harmonics even more than the former, yet at the cost of reduced efficiency. [ABSTRACT FROM AUTHOR]

An intense laser pulse in a plasma can accelerate electrons to GeV energies in centimetres. Transverse betatron motion in the plasma wake results in X-ray photons with an energy that depends on the electron energy, oscillation amplitude and frequency of the betatron motion. Betatron X-rays from laser-accelerator electrons have hitherto been limited to spectra peaking between 1 and 10?keV (ref. ). Here we show that the betatron amplitude is resonantly enhanced when electrons interact with the rear of the laser pulse. At high electron energy, resonance occurs when the laser frequency is a harmonic of the betatron frequency, leading to a significant increase in the photon energy. 108 gamma-ray photons, with spectra peaking between 20 and 150?keV, and a peak brilliance >1023?photons?s?1?mrad?2?mm?2 per 0.1% bandwidth, are measured for 700?MeV beams, with 107 photons emitted between 1 and 7?MeV. Femtosecond duration gamma-rays may find uses in imaging, isotope production, probing dense matter, homeland security and nuclear physics. [ABSTRACT FROM AUTHOR]

CO2 methanation is often performed on Ni/Al2O3 catalysts, which can suffer from mass transport limitations and, therefore, decreased efficiency. Here we show the application of a hierarchically porous Ni/Al2O3 catalyst for methanation of CO2. The material has a well-defined and connected meso- and macropore structure with a total porosity of 78%. The pore structure was thoroughly studied with conventional methods, i.e., N2 sorption, Hg porosimetry, and He pycnometry, and advanced imaging techniques, i.e., electron tomography and ptychographic X-ray computed tomography. Tomography can quantify the pore system in a manner that is not possible using conventional porosimetry. Macrokinetic simulations were performed based on the measures obtained by porosity analysis. These show the potential benefit of enhanced mass-transfer properties of the hierarchical pore system compared to a pure mesoporous catalyst at industrially relevant conditions. Besides the investigation of the pore system, the catalyst was studied by Rietveld refinement, diffuse reflectance ultraviolet-visible (DRUV/vis) spectroscopy, and H2-temperature programmed reduction (TPR), showing a high reduction temperature required for activation due to structural incorporation of Ni into the transition alumina. The reduced hierarchically porous Ni/Al2O3 catalyst is highly active in CO2 methanation, showing comparable conversion and selectivity for CH4 to an industrial reference catalyst. [ABSTRACT FROM AUTHOR]

X-ray ptychography has revolutionized nanoscale phase contrast imaging at large-scale synchrotron sources in recent years. We present here the first successful demonstration of the technique in a small-scale laboratory setting. An experiment was conducted with a liquid metal-jet x-ray source and a single photon-counting detector with a high spectral resolution. The experiment used a spot size of 5  μm to produce a ptychographic phase image of a Siemens star test pattern with a submicron spatial resolution. The result and methodology presented show how high-resolution phase contrast imaging can now be performed at small-scale laboratory sources worldwide. [ABSTRACT FROM AUTHOR]

X-ray microtomography is a nondestructive, three-dimensional inspection technique applied across a vast range of fields and disciplines, ranging from research to industrial, encompassing engineering, biology, and medical research. Phase-contrast imaging extends the domain of application of x-ray microtomography to classes of samples that exhibit weak attenuation, thus appearing with poor contrast in standard x-ray imaging. Notable examples are low-atomic-number materials, like carbon-fiber composites, soft matter, and biological soft tissues. We report on a compact and cost-effective system for x-ray phase-contrast microtomography. The system features high sensitivity to phase gradients and high resolution, requires a low-power sealed x-ray tube, a single optical element, and fits in a small footprint. It is compatible with standard x-ray detector technologies: in our experiments, we have observed that single-photon counting offered higher angular sensitivity, whereas flat panels provided a larger field of view. The system is benchmarked against known-material phantoms, and its potential for soft-tissue three-dimensional imaging is demonstrated on small-animal organs: a piglet esophagus and a rat heart. We believe that the simplicity of the setup we are proposing, combined with its robustness and sensitivity, will facilitate accessing quantitative x-ray phase-contrast microtomography as a research tool across disciplines, including tissue engineering, materials science, and nondestructive testing in general., Competing Interests: The authors declare no conflicts of interest., (Published by Optica Publishing Group under the terms of the Creative Commons Attribution 4.0 License. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.)

The characterisation of fast phenomena at the microscopic scale is required for the understanding of catastrophic responses of materials to loads and shocks, the processing of materials by optical or mechanical means, the processes involved in many key technologies such as additive manufacturing and microfluidics, and the mixing of fuels in combustion. Such processes are usually stochastic in nature and occur within the opaque interior volumes of materials or samples, with complex dynamics that evolve in all three dimensions at speeds exceeding many meters per second. There is therefore a need for the ability to record three-dimensional X-ray movies of irreversible processes with resolutions of micrometers and frame rates of microseconds. Here we demonstrate a method to achieve this by recording a stereo phase-contrast image pair in a single exposure. The two images are combined computationally to reconstruct a 3D model of the object. The method is extendable to more than two simultaneous views. When combined with megahertz pulse trains of X-ray free-electron lasers (XFELs) it will be possible to create movies able to resolve 3D trajectories with velocities of kilometers per second.

Cycloidal computed tomography provides high-resolution images within relatively short scan times by combining beam modulation with dedicated under-sampling. However, implementing the technique relies on accurate knowledge of the sample's motion, particularly in the case of continuous scans, which is often unavailable due to hardware or software limitations. We have developed an easy-to-implement position tracking technique using a sharp edge, which can provide reliable information about the trajectory of the sample and thus improve the reconstruction process. Furthermore, this approach also enables the development of other innovative sampling schemes, which may otherwise be difficult to implement.

Understanding catalyst deactivation by coking is crucial for knowledge-based catalyst and process design in reactions with carbonaceous species. Post-mortem analysis of catalyst coking is often performed by bulk characterization methods. Here, hard X-ray ptychographic computed tomography (PXCT) was used to study Ni/Al 2 O 3 catalysts for CO 2 methanation and CH 4 dry reforming after artificial coking treatment. PXCT generated quantitative 3D maps of local electron density at ca. 80 nm resolution, allowing to visualize and evaluate the severity of coking in entire catalyst particles of ca. 40 μm diameter. Coking was primarily revealed in the nanoporous solid, which was not detectable in resolved macropores. Coke formation was independently confirmed by operando Raman spectroscopy. PXCT is highlighted as an emerging characterization tool for nanoscale identification, co-localization, and potentially quantification of deactivation phenomena in 3D space within entire catalyst particles., (© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Due to complex degradation mechanisms, disparities between the theoretical and practical capacities of lithium-ion battery cathode materials persist. Specifically, Ni-rich chemistries such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (or NMC811) are one of the most promising choices for automotive applications; however, they continue to suffer severe degradation during operation that is poorly understood, thus challenging to mitigate. Here we use operando Bragg coherent diffraction imaging for 4D analysis of these mechanisms by inspecting the individual crystals within primary particles at various states of charge (SoC). Although some crystals were relatively homogeneous, we consistently observed non-uniform distributions of inter- and intracrystal strain at all measured SoC. Pristine structures may already possess heterogeneities capable of triggering crystal splitting and subsequently particle cracking. During low-voltage charging (2.7-3.5 V), crystal splitting may still occur even during minimal bulk deintercalation activity; and during discharging, rotational effects within parallel domains appear to be the precursor for the nucleation of screw dislocations at the crystal core. Ultimately, this discovery of the central role of crystal grain splitting in the charge/discharge dynamics may have ramifications across length scales that affect macroscopic performance loss during real-world battery operation.

Interest in phase contrast imaging methods based on electromagnetic wave coherence has increased significantly recently, particularly at X-ray energies. This is giving rise to a demand for effective simulation methods. Coherent imaging approaches are usually based on wave optics, which require significant computational resources, particularly for producing 2D images. Monte Carlo (MC) methods, used to track individual particles/photons for particle physics, are not considered appropriate for describing coherence effects. Previous preliminary work has evaluated the possibility of incorporating coherence in Monte Carlo codes. However, in this paper, we present the implementation of refraction in a model that is based on time of flight calculations and the Huygens-Fresnel principle, which allow reproducing the formation of phase contrast images in partially and fully coherent experimental conditions. The model is implemented in the FLUKA Monte Carlo code and X-ray phase contrast imaging simulations are compared with experiments and wave optics calculations.