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Scanning coherent X-ray microscopy (ptychography) has gained considerable interest during the last decade since the performance of this indirect imaging technique does not necessarily rely on the quality of the X-ray optics and, in principle, can achieve highest spatial resolution in X-ray imaging. The method can be easily extended to 3D by adding standard tomographic reconstruction schemes. However, the tomographic reconstruction is often applied in a subsequent step using a sequence of aligned ptychographic 2D projections. In this contribution, we outline current developments of a GPU-accelerated framework for direct 3D ptychography, coupling 2D ptychography and tomography. The program utilizes a custom GPU-accelerated framework for ptychography that offers three distinct ptychographic reconstruction algorithms. The tomographic reconstruction runs simultaneously and uses numerical routines of the ASTRA Toolbox. This parallel-computing approach results in a high performance increase considerably reducing the reconstruction time of 3D ptychographic datasets.

We demonstrate how the individual mirrors of a high-quality Kirkpatrick-Baez (KB) mirror system can be aligned to each other to create an optimally focused beam, through minimizing aberrations in the phase of the ptychographically reconstructed pupil function. Different sources of misalignment and the distinctive phase artifacts they create are presented via experimental results from the alignment of the KB mirrors at the NanoMAX diffraction endstation. The catalog of aberration artifacts can be used to easily identify which parameter requires further tuning in the alignment of any KB mirror system.

The coherence properties of the beam provided at the CoSAXS beamline at the MAX IV Laboratory are determined experimentally using multi-mode ptychography. The coherent fraction of the beam is then used for a proof-of-concept XPCS measurement, illustrating the beamline’s capabilities., The CoSAXS beamline at the MAX IV Laboratory is a modern multi-purpose (coherent) small-angle X-ray scattering (CoSAXS) instrument, designed to provide intense and optionally coherent illumination at the sample position, enabling coherent imaging and speckle contrast techniques. X-ray tracing simulations used to design the beamline optics have predicted a total photon flux of 1012–1013 photons s−1 and a degree of coherence of up to 10% at 7.1 keV. The normalized degree of coherence and the coherent flux of this instrument were experimentally determined using the separability of a ptychographic reconstruction into multiple mutually incoherent modes and thus the Coherence in the name CoSAXS was verified. How the beamline can be used both for coherent imaging and XPCS measurements, which both heavily rely on the degree of coherence of the beam, was demonstrated. These results are the first experimental quantification of coherence properties in a SAXS instrument at a fourth-generation synchrotron light source.

Contrast, a simple Python framework for controlling beamline experiments, is presented. Contrast can be easily adapted to any beamline, or serve as inspiration for constructing new, suitable tools tailored to individual instruments., The emergence of fourth-generation synchrotrons is prompting the development of new systems for experimental control and data acquisition. However, as general control systems are designed to cover a wide set of instruments and techniques, they tend to become large and complicated, at the cost of experimental flexibility. Here we present Contrast, a simple Python framework for interacting with beamline components, orchestrating experiments and managing data acquisition. The system is presented and demonstrated via its application at the NanoMAX beamline of the MAX IV Laboratory.

Ptychographic X-ray computed tomography is a quantitative three-dimensional imaging technique offered to users of multiple synchrotron radiation sources. Its dependence on the coherent fraction of the available X-ray beam makes it perfectly suited to diffraction-limited storage rings. Although MAX IV is the first, and so far only, operating fourth-generation synchrotron light source, none of its experimental stations is currently set up to offer this technique to its users. The first ptychographic X-ray computed tomography experiment has therefore been performed on the NanoMAX beamline. From the results, information was gained about the current limitations of the experimental setup and where attention should be focused for improvement. The extracted parameters in terms of scanning speed, size of the imaged volume and achieved resolutions should provide a baseline for future users designing nano-tomography experiments on the NanoMAX beamline.

X-ray fluorescence microscopy performed at nanofocusing synchrotron beamlines produces quantitative elemental distribution maps at unprecedented resolution (down to a few tens of nanometres), at the expense of relatively long measuring times and high absorbed doses. In this work, a method was implemented in which fast low-dose in-line holography was used to produce quantitative electron density maps at the mesoscale prior to nanoscale X-ray fluorescence acquisition. These maps ensure more efficient fluorescence scans and the reduction of the total absorbed dose, often relevant for radiation-sensitive (e.g. biological) samples. This multimodal microscopy approach was demonstrated on human sural nerve tissue. The two imaging modes provide complementary information at a comparable resolution, ultimately limited by the focal spot size. The experimental setup presented allows the user to swap between them in a flexible and reproducible fashion, as well as to easily adapt the scanning parameters during an experiment to fine-tune resolution and field of view.

The diffraction endstation of the NanoMAX beamline is designed to provide high-flux coherent X-ray nano-beams for experiments requiring many degrees of freedom for sample and detector. The endstation is equipped with high-efficiency Kirkpatrick–Baez mirror focusing optics and a two-circle goniometer supporting a positioning and scanning device, designed to carry a compact sample environment. A robot is used as a detector arm. The endstation, in continued development, has been in user operation since summer 2017.

Journal of synchrotron radiation 26(5), 1769 - 1781 (2019). doi:10.1107/S160057751900660X, Two in situ `nanoreactors' for high-resolution imaging of catalysts have been designed and applied at the hard X-ray nanoprobe endstation at beamline P06 of the PETRA III synchrotron radiation source. The reactors house samples supported on commercial MEMS chips, and were applied for complementary hard X-ray ptychography (23 nm spatial resolution) and transmission electron microscopy, with additional X-ray fluorescence measurements. The reactors allow pressures of 100 kPa and temperatures of up to 1573 K, offering a wide range of conditions relevant for catalysis. Ptychographic tomography was demonstrated at limited tilting angles of at least ±35° within the reactors and ±65° on the naked sample holders. Two case studies were selected to demonstrate the functionality of the reactors: (i) annealing of hierarchical nanoporous gold up to 923 K under inert He environment and (ii) acquisition of a ptychographic projection series at ±35° of a hierarchically structured macroporous zeolite sample under ambient conditions. The reactors are shown to be a flexible and modular platform for in situ studies in catalysis and materials science which may be adapted for a range of sample and experiment types, opening new characterization pathways in correlative multimodal in situ analysis of functional materials at work. The cells will presently be made available for all interested users of beamline P06 at PETRA III., Published by IUCr, Chester

This work is an overview of the multi-modal hard X-ray nanoprobe beamline at the MAX IV Laboratory. The beamline provides an intense and coherent beam, focused to 40–200 nm in the energy range 5–28 eV., NanoMAX is the first hard X-ray nanoprobe beamline at the MAX IV laboratory. It utilizes the unique properties of the world’s first operational multi-bend achromat storage ring to provide an intense and coherent focused beam for experiments with several methods. In this paper we present the beamline optics design in detail, show the performance figures, and give an overview of the surrounding infrastructure and the operational diffraction endstation.

First results of in-line holography and holotomography from the NanoMAX beamline at MAX IV are presented., Coherent X-ray imaging techniques, such as in-line holography, exploit the high brilliance provided by diffraction-limited storage rings to perform imaging sensitive to the electron density through contrast due to the phase shift, rather than conventional attenuation contrast. Thus, coherent X-ray imaging techniques enable high-sensitivity and low-dose imaging, especially for low-atomic-number (Z) chemical elements and materials with similar attenuation contrast. Here, the first implementation of in-line holography at the NanoMAX beamline is presented, which benefits from the exceptional focusing capabilities and the high brilliance provided by MAX IV, the first operational diffraction-limited storage ring up to approximately 300 eV. It is demonstrated that in-line holography at NanoMAX can provide 2D diffraction-limited images, where the achievable resolution is only limited by the 70 nm focal spot at 13 keV X-ray energy. Also, the 3D capabilities of this instrument are demonstrated by performing holotomography on a chalk sample at a mesoscale resolution of around 155 nm. It is foreseen that in-line holography will broaden the spectra of capabilities of MAX IV by providing fast 2D and 3D electron density images from mesoscale down to nanoscale resolution.

Applied physics letters 118(17), 171102 (1-5) (2021). doi:10.1063/5.0045571, Nondestructive imaging with both a large field of view and a high spatial resolution is crucial to understand complex materials and processes in science and technology. X-ray ptychography can provide highest spatial resolution but is limited in the field of view by the acquisition time and coherent flux at modern x-ray sources. By multi-beam ptychography, the sample can be imaged in parallel by several spatially separated and mutually incoherent beams. We have implemented this method using 3D nanoprinted x-ray optics to create tailor-made x-ray multi-beam arrays. The use of 3D printing allows us to create focusing optics with a minimum of nonfunctional support structures. In this way, large sample areas can be efficiently scanned in parallel with up to six illuminating beams., Published by American Inst. of Physics, Melville, NY

The NanoMAX hard X-ray nanoprobe is the first beamline to take full advantage of the diffraction-limited storage ring at the MAX IV synchrotron and delivers a high coherent photon flux for applications in diffraction and imaging. Here, we characterize its coherent and focused beam using ptychographic analysis. We derive beam profiles in the energy range 6-22 keV and estimate the coherent flux based on a probe mode decomposition approach.

For decades, Cu has been the primary dopant in CdTe photovoltaic absorbers. Typically, Cu acceptor concentrations in these devices are on the order of 1 × 1014 cm−3, which has made it notoriously difficult to directly correlate nanoscale Cu distributions to the local charge transport properties of these devices. To measure and correlate these properties, measurement techniques require high sensitivity to elemental concentration, large penetration depth, and operando compatibility. Techniques such as secondary-ion mass spectroscopy and X-ray energy dispersive spectroscopy are widely adopted to measure Cu concentrations, but they are limited by penetration depth, sensitivity, or spatial resolution. Additionally, they lack the operando capabilities required to correlate one-to-one Cu concentrations to electrical performance. In this work, correlative X-ray microscopy is used to investigate the spatial distribution of Cu and its impact on charge collection through the depth and breadth of CdTe photovoltaic devices. Plan-view, nanoscale X-ray fluorescence maps clearly demonstrate the spatial segregation of copper around regions thought to be CdTe grain boundaries. Complementary cross-section imaging unveils the transition of the maximum charge-collection efficiency from the ZnTe–CdTe interface to the CdS–CdTe interface as a function of Cu incorporation. The copper concentration through the depth of the CdTe layer is characterized by slow and fast diffusion components, and cross-section charge-transport modeling shows that the experimentally obtained charge collection can be explained by the modeled acceptor distribution through the depth of the CdTe layer.

Journal of synchrotron radiation 27(5), 1121 - 1130 (2020). doi:10.1107/S1600577520007900, Modern subtractive and additive manufacturing techniques present new avenues for X-ray optics with complex shapes and patterns. Refractive phase plates acting as glasses for X-ray optics have been fabricated, and spherical aberration in refractive X-ray lenses made from beryllium has been successfully corrected. A diamond phase plate made by femtosecond laser ablation was found to improve the Strehl ratio of a lens stack with a numerical aperture (NA) of 0.88 × 10−3 at 8.2 keV from 0.1 to 0.7. A polymer phase plate made by additive printing achieved an increase in the Strehl ratio of a lens stack at 35 keV with NA of 0.18 × 10−3 from 0.15 to 0.89, demonstrating diffraction-limited nanofocusing at high X-ray energies., Published by Wiley-Blackwell, [S.l.]

Journal of synchrotron radiation 27(2), 486 - 493 (2020). doi:10.1107/S1600577520000831, This paper presents a deep learning algorithm for tomographic reconstruction(GANrec). The algorithm uses a generative adversarial network (GAN) to solvethe inverse of the Radon transform directly. It works for independent sinogramswithout additional training steps. The GAN has been developed to fit the inputsinogram with the model sinogram generated from the predicted reconstruction.Good quality reconstructions can be obtained during the minimization of thefitting errors. The reconstruction is a self-training procedure based on thephysics model, instead of on training data. The algorithm showed significantimprovements in the reconstruction accuracy, especially for missing-wedgetomography acquired at less than 180 rotational range. It was also validatedby reconstructing a missing-wedge X-ray ptychographic tomography (PXCT)data set of a macroporous zeolite particle, for which only 51 projections over70 could be collected. The GANrec recovered the 3D pore structure withreasonable quality for further analysis. This reconstruction concept can workuniversally for most of the ill-posed inverse problems if the forward model iswell defined, such as phase retrieval of in-line phase-contrast imaging., Published by Wiley-Blackwell, [S.l.]

Journal of applied crystallography 53(4), 957 - 971 (2020). doi:10.1107/S1600576720008420, Ptychographic X-ray imaging at the highest spatial resolution requires an optimal experimental environment, providing a high coherent flux, excellent mechanical stability and a low background in the measured data. This requires, for example, a stable performance of all optical components along the entire beam path, high temperature stability, a robust sample and optics tracking system, and a scatter-free environment. This contribution summarizes the efforts along these lines to transform the nanoprobe station on beamline P06 (PETRA III) into the ptychographic nano-analytical microscope (PtyNAMi)., Published by Wiley-Blackwell, [S.l.]

Journal of synchrotron radiation 28(3), 1030 (2021). doi:10.1107/S1600577521003167, A correction in the paper by Seiboth et al. [(2018). J. Synchrotron Rad. 25, 108���115] is made., Published by Wiley-Blackwell, [S.l.]

Optics letters 44(18), 4622 - 4625 (2019). doi:10.1364/OL.44.004622, In this Letter, we report on the creation of hard x-ray beams carrying orbital angular momentum of topological charge $−ℏ$ and $−3ℏ$ at a photon energy of 8.2 keV via spiral phase plates made out of fused silica by ultrashort-pulsed laser ablation. The phase plates feature a smooth phase ramp with a 0.5 μm nominal step height and a surface roughness of 0.5 μm. The measured vortex beams show submicrometer-sized donut rings and agree well with numerical modeling. Fused silica phase plates are potentially suited to manipulate the electromagnetic field in highly intense x-ray beams at x-ray free-electron laser sources., Published by OSA, Washington, DC

Optica 6(10), 1282 -1289 (2019). doi:10.1364/OPTICA.6.001282, Three-dimensional (3D) x-ray microscopy by ptychographic tomography requires elaborate numerical reconstructions. We describe a coupled ptychography-tomography reconstruction algorithm and apply it to an experimental ptychographic x-ray computed tomography data set of a catalyst particle. Compared to the traditional sequential algorithm, in which ptychographic projections are reconstructed to serve as input for subsequent tomographic reconstruction, the coupled ptychography-tomography algorithm reconstructs the 3D volume with higher spatial resolution over a larger field of view. Coupling the data from different projections improves the overall reconstruction, and the ptychographic sampling in individual projections can be coarsened beyond the point of overlap between neighboring scan points, still leading to stable reconstructions., Published by OSA, Washington, DC

X-Ray Nanoimaging: Instruments and Methods IV, San Diego, United States, 11 Aug 2019 - 15 Aug 2019; Proceedings of SPIE 11112, 111120D-1 (2019). doi:10.1117/12.2529096, The X-ray scanning microscope PtyNAMi at beamline P06 of PETRA III at DESY in Hamburg, Germany, isdesigned for high-spatial-resolution 3D imaging with high sensitivity. Besides optimizing the coherent ux densityon the sample and the precision mechanics of the scanner, special care has been taken to reduce backgroundsignals on the detector. The optical path behind the sample is evacuated up until the sensor of a four-megapixeldetector that is placed into the vacuum. In this way, parasitic scattering from air and windows close to thedetector is avoided. The instrument has been commissioned and is in user operation. The main commissioningresults of the low-background detector system are presented. A signal-to-noise model for small object details isderived that includes incoherent background scattering, Published by SPIE, Bellingham, Wash.

Chemistry - a European journal 25, 14430-14440 (2019). doi:10.1002/chem.201903287, We report the successful synthesis of hierarchically structuredtitanium silicalite-1 (TS-1) with large intracrystalline macroporesby steam-assisted crystallisation of mesoporous silica particles.The macropore topology was imaged in 3D using electrontomography and synchrotron radiation-based ptychographic Xraycomputed tomography, revealing interconnectedmacropores within the crystals accounting for about 30 % of theparticle volume. The study of the macropore formationmechanism revealed that the mesoporous silica particles act asa sacrificial macropore template during the synthesis. Silicon totitanium ratio of the macroporous TS-1 samples wassuccessfully tuned from 100 to 44. The hierarchically structuredTS-1 exhibited high activity in the liquid phase epoxidation of 2-octene with hydrogen peroxide. The hierarchically structured TS-1 surpassed a conventional nano-sized TS-1 sample in terms ofalkene conversion and showed comparable selectivity to theepoxide. The flexible synthesis route described here can be usedto prepare hierarchical zeolites with improved mass transportproperties for other selective oxidation reactions., Published by Wiley-VCH, Weinheim

X-Ray Microscopy 2018, Saskatoon, Canada, 19 Aug 2018 - 24 Aug 2018; Microscopy and microanalysis 24(S2), 434 - 435 (2018). doi:10.1017/S1431927618014423, Published by Cambridge University Press

Nanofocus x-ray diffraction is used to investigate the structure and local strain field of an isolated ðIn; GaÞN=GaN core-shell microrod. Because the high spatial resolution of the x-ray beam is only 80 × 90 nm2, we are able to investigate several distinct volumes on one individual side facet. Here, we find a drastic increase in thickness of the outer GaN shell along the rod height. Additionally, we performed highangle annular dark-field scanning-transmission-electron-microscopy measurements on several rods from the same sample showing that (In,Ga)N double-quantum-well and GaN barrier thicknesses also increase strongly along the height. Moreover, plastic relaxation is observed in the top part of the rod. Based on the experimentally obtained structural parameters, we simulate the strain-induced deformation using the finiteelement method, which serves as the input for subsequent kinematic scattering simulations. The simulations reveal a significant increase of elastic in-plane relaxation along the rod height. However, at a certain height, the occurrence of plastic relaxation yields a decrease of the elastic strain. Because of the experimentally obtained structural input for the finite-element simulations, we can exclude unknown structural influences on the strain distribution, and we are able to translate the elastic relaxation into an indium concentration which increases by a factor of 4 from the bottom to the height where plastic relaxation occurs.

SPIE OPTICAL ENGINEERING + APPLICATIONS | 6-10 AUGUST 2017; X-Ray Nanoimaging: Instruments and Methods III X-Ray Nanoimaging: Instruments and Methods III, San Diego, United States, 6 Aug 2017 - 10 Aug 2017; Proceedings of SPIE 10389, 1038901 (2017). doi:10.1117/12.2273710, In recent years, ptychography has revolutionized x-ray microscopy in that it is able to overcome the diffraction limit of x-ray optics, pushing the spatial resolution limit down to a few nanometers. However, due to the weak interaction of x rays with matter, the detection of small features inside a sample requires a high coherent fluence on the sample, a high degree of mechanical stability, and a low background signal from the x-ray microscope. The x-ray scanning microscope PtyNAMi at PETRA III is designed for high-spatial-resolution 3D imaging with high sensitivity. The design concept is presented with a special focus on real-time metrology of the sample position during tomographic scanning microscopy., Published by SPIE, Bellingham, Wash.

SPIE Optical Engineering + Applications, San Diego, California ; Proceedings of SPIE 9963, 99630P(2016). doi:10.1117/12.2237646, Due to the weak interaction of X-rays with matter and their small wavelength on the atomic scale, stringent requirements are put on X-ray optics manufacturing and metrology. As a result, these optics often suffer from aberrations. Until now, X-ray optics were mainly characterized by their focal spot size and efficiency. How- ever, both measures provide only insufficient information about optics quality. Here, we present a quantitative analysis of residual aberrations in current beryllium compound refractive lenses using ptychography followed by a determination of the wavefront error and subsequent Zernike polynomial decomposition. Known from visible light optics, we show that these measures can provide an adequate tool to determine and compare the quality of various X-ray optics., Published by SPIE, Bellingham, Wash.

The hard x-ray scanning microscope at beamline P06 of PETRA III at DESY in Hamburg serves a large user community, from physics, chemistry, and nanotechnology to the bio-medical, materials, environmental, and geosciences. It has been in user operation since 2012, and is mainly based on nanofocusing refractive x-ray lenses. Using refractive optics, nearly gaussian-limited nanobeams in the range from 50 to 100 nm can be generated in the hard x-ray energy range from 8 to 30 keV. The degree of coherence can be traded off against the flux in the nanobeam by a two-stage focusing scheme. We give a brief overview on published results from this instrument and describe its most important components and parameters.