Diffraction Imaging Techniques Research Articles

Fast X-ray ptychography: towards nanoscale imaging of large volume of brain

X-ray ptychography, a scanning coherent diffraction imaging technique, is one of the most used techniques at synchrotron facilities for high resolution imaging, with applications spanning from life science to nano-electronics. In the recent years there has been a great effort to make the technique faster to enable high throughput nanoscale imaging. Here we apply a fast ptychography scanning method to image in 3D 106μm3\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$10^6\\upmu \\mathrm{{m}}^3$$\\end{document} of brain-like phantom at 3 kHz, in a 7 h acquisition with a resolution of 270 nm. We then present the latest advances in fast ptychography by showing 2D images acquired at 110 kHz by combining the fast-acquisition scheme with a high-acquisition rate prototype detector from DECTRIS Ltd. We finally review the experimental outcome and discuss the prospective use of fast ptychography schemes for the investigation of mm3\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{3}$$\\end{document} size samples of brain-like phantom, by extrapolating the current results to the high coherent flux scenario of diffraction limited storage rings.

Revealing the inhomogeneous nature of microstructure and texture evolution in the cold-rolled CoCrFeMnNi alloy during static recrystallization

In the present investigation, equiatomic CoCrFeMnNi high entropy alloy (HEA) was subjected to 80% cold rolling (as-rolled) followed by isothermal annealing treatment at 700 °C for different time periods. Microstructural characterization was performed using electron back-scattered diffraction (EBSD) and electron channeling contrast imaging (ECCI) techniques on the as-rolled and annealed samples. The as-rolled microstructure consisted of elongated grains mainly composed of strong α-fiber and weak γ-fiber textures. The as-rolled sample showed the formation of ingrain SBs in the γ-fiber grains, which served as preferential sites for grain nucleation. The annealing treatment of as-rolled samples at 700 °C cause static recovery (SRV) before 5 minutes of heat-treatment, whereas static recrystallization (SRX) was observed after 5 minutes of heat-treatment in the CoCrFeMnNi alloy samples. A faster rate of recrystallization kinetics was observed after 15 minutes of heat-treatment. The annealing treatment reduced the intensity of α-fiber and enhanced the Copper, Cube and P ({011}<122>) texture components. Copper components originated from coarse recrystallized grains, which were the results of localized grain growth phenomena. Unusual behavior of banded featured α-fiber grains was observed during the annealing process. These banded grains in the partially annealed samples consisted of subgrain-boundaries and showed a delayed response to recrystallization as compared to grains with other orientations. Stored energy (SE) and Taylor factor (M) calculations were also used to understand the delayed recrystallization response of the banded featured/retained deformed grains. The microhardness value of the as-rolled sample was approximately 450 Hv, which decreased to around 230 Hv for the fully recrystallized grains.

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

Emergent Three-Dimensional Electric Dipole Sinewave in Bulk Perovskite Oxides.

The magnetic and electric dipoles of ferroics play a central role in their fascinating properties. In particular, topological configurations have shown promising potential for use in novel electromechanical and electronic devices. Magnetic configurations from simple collinear to complex topological are well-documented. In contrast, many complex topological features in the electric counterpart remain unexplored. Here, we report the first example of three-dimensional electric dipole sinewave topological structure in a PbZrO3-based bulk perovskite, which presents an interesting triple-hysteresis loop macroscopically. This polar configuration consists of two orthogonal sinewave electric dipole modulations decoded from a polar incommensurate phase by advanced diffraction and atomic-resolution imaging techniques. The resulting topology is unraveled to be the competition between the antiferroelectric and ferroelectric states, stabilized by the modulation of the Pb 6s2 lone pair and the antiferrodistortive effect. These findings further reinforce the similarity of the magnetic and electric topologies.

ProSPyX: software for post-processing images of X-ray ptychography with spectral capabilities.

X-ray ptychography is a coherent diffraction imaging technique based on acquiring multiple diffraction patterns obtained through the illumination of the sample at different partially overlapping probe positions. The diffraction patterns collected are used to retrieve the complex transmittivity function of the sample and the probe using a phase retrieval algorithm. Absorption or phase contrast images of the sample as well as the real and imaginary parts of the probe function can be obtained. Furthermore, X-ray ptychography can also provide spectral information of the sample from absorption or phase shift images by capturing multiple ptychographic projections at varying energies around the resonant energy of the element of interest. However, post-processing of the images is required to extract the spectra. To facilitate this, ProSPyX, a Python package that offers the analysis tools and a graphical user interface required to process spectral ptychography datasets, is presented. Using the PyQt5 Python open-source module for development and design, the software facilitates extraction of absorption and phase spectral information from spectral ptychographic datasets. It also saves the spectra in file formats compatible with other X-ray absorption spectroscopy data analysis software tools, streamlining integration into existing spectroscopic data analysis pipelines. To illustrate its capabilities, ProSPyX was applied to process the spectral ptychography dataset recently acquired on a nickel wire at the SWING beamline of the SOLEIL synchrotron.

Dose symmetric electron diffraction tomography (DS-EDT): Implementation of a dose-symmetric tomography scheme in 3D electron diffraction

Beam sensitive nanomaterials such as zeolites or metal-organic frameworks (MOF) represent a great challenge for crystallographic structure determination and refinement. The strong electron-matter interaction and the high spatial resolution achievable make electron diffraction the technique of choice for particles of sizes below a micrometer and many different 3-dimensional electron diffraction (3D ED) techniques have been developed in recent years. Nevertheless, beam sensitivity of the samples can lead to the crystal structure being damaged during the data acquisition impeding the determination of its structure. A simple way to reduce beam damage is to lower the dose during the experiment. However, this implies weaker diffraction intensities which can become problematic for the exploitation of the data.In order to obtain complete data sets with strong intensities without damaging the crystals, we developed the dose symmetric electron diffraction tomography (DS-EDT) method, combining the low-dose electron diffraction tomography (LD-EDT) technique with the dose-symmetric tomography scheme known from cryo-EM. In order to reduce the dose on an individual crystal and still obtain enough data for a structure solution and refinement, we partition the dose over several crystals. The individual datasets are then merged in order to achieve the necessary completeness. On two test structures we first show that merging of data from small domains of the reciprocal space is indeed sufficient to obtain reliable data for structure solution and refinement. Second, we show on the beam sensitive manganese formate that high-quality data can be obtained on a few frames while the frames that have suffered from beam damage can still be used to determine the orientation matrix and the unit cell of the crystals. The results from the dynamical refinement on the obtained data show a high accuracy of the atom positions. In this way, DS-EDT can reduce the total dose on an individual crystal by an order of magnitude with respect to the already very dose-efficient LD-EDT.

An advanced Bragg diffraction imaging technique to characterize defects: The examples of GaN and AlN

An advanced X-ray Bragg diffraction imaging technique known as Rocking Curve Imaging (RCI) was implemented and developed at the European Synchrotron Radiation Facility (ESRF), where it complements the simpler and faster, but less accurate, “white beam topography” technique. These techniques allow the observation and characterization of defects in bulk crystals, as well as in crystalline layers with a thickness in the μm range. We recall the basics of X-ray Bragg diffraction imaging (historically called X-ray topography) and describe the technical aspects of RCI, including the approximations we often use to analyse the images, and the information we can extract from the various produced maps (Integrated Intensity, Full Width Half Maximum and Peak Position). We show, as examples, results of its application to aluminium nitride (AlN) and gallium nitride (GaN) crystals that are used as substrates for microelectronic devices. More in particular we describe the images of individual dislocations in crystals of both materials, and the particular arrangement of threading dislocations in ammonothermally grown GaN that lead to subgrain boundaries and hexagonal shaped (“honeycomb”) defects. These examples show that the RCI Bragg diffraction imaging technique allows obtaining unique results, in the sub-μm spatial resolution and the μradian range angular resolution ranges, when the characterization of high-quality crystals is required.

Darfix - data analysis for dark-field X-ray microscopy.

A Python package for the analysis of dark-field X-ray microscopy (DFXM) and rocking curve imaging (RCI) data is presented. DFXM is a non-destructive diffraction imaging technique that provides three-dimensional maps of lattice strain and orientation. The darfix package enables fast processing and visualization of these data, providing the user with the essential tools to extract information from the acquired images in a fast and intuitive manner. These data processing and visualization tools can be either imported as library components or accessed through a graphical user interface as an Orange add-on. In the latter case, the different analysis modules can be easily chained to define computational workflows. Operations on larger-than-memory image sets are supported through the implementation of online versions of the data processing algorithms, effectively trading performance for feasibility when the computing resources are limited. The software can automatically extract the relevant instrument angle settings from the input files' metadata. The currently available input file format is EDF and in future releases HDF5 will be incorporated.

Development and applications ofultrafast transmission electron microscopy.

We present a review on the development and applications of the ultrafast transmission electron microscopy (UTEM) at RIKEN. We introduce the UTEM system for the pump-probe TEM observation in a wide temporal range. By combining the UTEM and pixelated detector, we further develop five-dimansional scanning TEM (5D STEM) which provides the ultrafast nanoscale movie of physical quantities in nano-materials, such as crystal lattice information and electromagnetic field, by convergent-beam electron diffraction (CBED) and differential phase contrast (DPC) imaging technique. We show our recent results on the nanosecond-to-microsecond magnetic skyrmion dynamics observed by Lorentz TEM (LTEM) and photo-induced acoustic wave generation in picosecond regime by bright-field TEM and electron diffraction measurements by UTEM. We also show the demonstartion of the 5D STEM on the quantitative time (t)-dependent strain mapping by CBED with an accuracy of 4 ps and 8 nm, and the ultrafast demagnetization under zero magnetic field observed by DPC with 10 ns and 400 nm resolution.

Thermus thermophilus polyploid cells directly imaged by X-ray laser diffraction.

Thermus thermophilus is reportedly polyploid and carries four to five identical genome copies per cell, based on molecular biological experiments. To directly detect polyploidy in this bacterium, we performed live cell imaging by X-ray free-electron laser (XFEL) diffraction and observed its internal structures. The use of femtosecond XFEL pulses enables snapshots of live, undamaged cells. For successful XFEL imaging, we developed a bacterial culture method using a starch- and casein-rich medium that produces a predominance of rod-shaped cells shorter than the focused XFEL beam size, which is slightly smaller than 2 µm. When cultured in the developed medium, the length of T. thermophilus cells, which is typically ~4 µm, was less than half its usual length. We placed living cells in a micro-liquid enclosure array and successively exposed each enclosure to a single XFEL pulse. A cell image was successfully obtained by the coherent diffractive imaging technique with iterative phase retrieval calculations. The reconstructed cell image revealed five peaks, which are most likely to be nucleoids, arranged in a row in the polyploid cell without gaps. This study demonstrates that XFELs offer a novel approach for visualizing the internal nanostructures of living, micrometer-sized, polyploid bacterial cells.

Damage-Free Femtosecond X-Ray Laser Snapshot Imaging of Catalyst Layer Nano-Structures of Polymer Electrolyte Fuel Cells

The realization of the hydrogen society, where hydrogen is used as clean and renewable energy, is desired to reduce carbon dioxide emissions and achieve sustainable development. The polymer electrolyte fuel cell (PEFC) is a key technology for automobiles in the hydrogen society as an alternative to conventional internal combustion engines. However, further improvements in PEFC performances are required for the full-scale spread of fuel cell vehicles. This study aims to image the nanostructures of the catalyst layer, which is particularly important in determining the performance of PEFCs, and correlate the observed structures with mass transfer in the catalyst layer. The catalyst layer contains catalyst-loaded carbon supports thinly covered with an ionomer responsible for proton conduction. We are especially interested in observing the support structure and ionomer coverage.We performed coherent X-ray imaging studies on the catalyst particles of PEFCs using an X-ray free-electron laser (XFEL) facility: SACLA (SPring-8 Angstrom Compact free electron LAser). Femtosecond XFEL allows us to capture radiation-damage-free snapshot images by outrunning major radiation damage processes. Damage-free imaging is of great value because radiation damage often causes a problem in high-resolution electron microscopy observation of ionomers. We used the coherent diffractive imaging (CDI) technique to observe catalyst particles of PEFCs. In CDI, sample images are reconstructed from measured coherent diffraction patterns using phase-retrieval calculation instead of objective lenses. CDI enables quantitative phase imaging and allows high-contrast imaging of the catalyst particles, which are almost transparent to X-rays.The measurement was carried out for catalyst particles in the dried condition and in solution. Our study showed that the image contrast can be adjusted by changing the electron density of the volume surrounding the sample1). The dried sample was prepared by dropping catalyst ink onto a silicon nitride membrane and air-dried. The solution sample was enclosed in micro-liquid enclosure arrays2,3) developed at Hokkaido University. The coherent diffraction patterns were measured by irradiating the sample catalyst particles with the 100-nm-focused XFEL beam with a photon energy of 4 keV using MAXIC-S (Multiple Application X-ray Imaging Chamber-S)4). The phase-retrieval calculation reconstructed the sample images. Fig. 1 shows a reconstructed image of a catalyst particle in water. The reconstructed image shows many white spots, which can be interpreted as platinum-cobalt catalysts. The pixel size of the reconstructed image is 1.3 nm, demonstrating among the highest spatial resolution in X-ray imaging. We will continue our study to observe the support structures and their ionomer coverage to understand the mass transfer in the catalyst layer.This work was supported by the FC-Platform of NEDO (New Energy and Industrial Technology Development Organization). The XFEL experiments were performed at SACLA with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal Nos. 2020A8106, 2021A8010, and 2021B8019).

Π-Net: A double-branch network framework for scanning coherent diffraction imaging

Ptychography is a coherent diffractive imaging technique that surpasses the resolution limitations of typical X-ray optics. It generates label-free, high-contrast quantitative amplitude and phase images without requiring prior knowledge. How to quickly recover high-fidelity amplitude and phase contrast images of an authentic sample is a challenge, however, due to the expensive computation that precludes real-time imaging. This paper proposes a framework with a double-branch network, Π-Net, to solve this complex problem. It can simultaneously and robustly reconstruct the object's phase and amplitude information from a degraded image. By analyzing the performance of various activation functions, we find that the activation function plays a crucial role in phase retrieval. Numerical experiments demonstrate the robustness of Π-Net, and our reconstruction results are superior to those of state-of-the-art methods. In addition, ablation studies have revealed that the negative output of neurons can contribute to improved reconstruction outcomes.

Coherent modulation imaging using a physics-driven neural network.

Coherent modulation imaging (CMI) is a lessness diffraction imaging technique, which uses an iterative algorithm to reconstruct a complex field from a single intensity diffraction pattern. Deep learning as a powerful optimization method can be used to solve highly ill-conditioned problems, including complex field phase retrieval. In this study, a physics-driven neural network for CMI is developed, termed CMINet, to reconstruct the complex-valued object from a single diffraction pattern. The developed approach optimizes the network's weights by a customized physical-model-based loss function, instead of using any ground truth of the reconstructed object for training beforehand. Simulation experiment results show that the developed CMINet has a high reconstruction quality with less noise and robustness to physical parameters. Besides, a trained CMINet can be used to reconstruct a dynamic process with a fast speed instead of iterations frame-by-frame. The biological experiment results show that CMINet can reconstruct high-quality amplitude and phase images with more sharp details, which is practical for biological imaging applications.

Single-shot ptychography at a soft X-ray free-electron laser

In this work, single-shot ptychography was adapted to the XUV range and, as a proof of concept, performed at the free-electron laser FLASH at DESY to obtain a high-resolution reconstruction of a test sample. Ptychography is a coherent diffraction imaging technique capable of imaging extended samples with diffraction-limited resolution. However, its scanning nature makes ptychography time-consuming and also prevents its application for mapping of dynamical processes. Single-shot ptychography can be realized by collecting the diffraction patterns of multiple overlapping beams in one shot and, in recent years, several concepts based on two con-focal lenses were employed in the visible regime. Unfortunately, this approach cannot be extended straightforwardly to X-ray wavelengths due to the use of refractive optics. Here, a novel single-shot ptychography setup utilizes a combination of X-ray focusing optics with a two-dimensional beam-splitting diffraction grating. It facilitates single-shot imaging of extended samples at X-ray wavelengths.

Quantitative, in situ visualization of intracellular insulin vesicles in pancreatic beta cells

Characterizing relationships between Zn2+, insulin, and insulin vesicles is of vital importance to the study of pancreatic beta cells. However, the precise content of Zn2+ and the specific location of insulin inside insulin vesicles are not clear, which hinders a thorough understanding of the insulin secretion process and diseases caused by blood sugar dysregulation. Here, we demonstrated the colocalization of Zn2+ and insulin in both single extracellular insulin vesicles and pancreatic beta cells by using an X-ray scanning coherent diffraction imaging (ptychography) technique. We also analyzed the elemental Zn2+ and Ca2+ contents of insulin vesicles using electron microscopy and energy dispersive spectroscopy (EDS) mapping. We found that the presence of Zn2+ is an important characteristic that can be used to distinguish insulin vesicles from other types of vesicles in pancreatic beta cells and that the content of Zn2+ is proportional to the size of insulin vesicles. By using dual-energy contrast X-ray microscopy and scanning transmission X-ray microscopy (STXM) image stacks, we observed that insulin accumulates in the off-center position of extracellular insulin vesicles. Furthermore, the spatial distribution of insulin vesicles and their colocalization with other organelles inside pancreatic beta cells were demonstrated using three-dimensional (3D) imaging by combining X-ray ptychography and an equally sloped tomography (EST) algorithm. This study describes a powerful method to univocally describe the location and quantitative analysis of intracellular insulin, which will be of great significance to the study of diabetes and other blood sugar diseases.

X-ray diffraction imaging of the diamond anvils based on the microfocus x-ray source with a liquid anode.

This paper presents the results of using laboratory x-ray systems in the study of the crystal structure of anvil made from single-crystal diamond. The system is equipped with an Excillum MetalJet D2 + 70kV high-brightness x-ray source with a liquid GaIn anode. The x-ray diffraction imaging (topography) technique with the use of a high-resolution x-ray Rigaku camera was applied to analyze crystal structure defects. Two-dimensional images were experimentally recorded using 400 and 111 reflections with a resolution of 1.5 and 5μm, respectively. These topograms displayed various defects, such as growth striations and dislocations. Possible applications of the proposed laboratory-based optical scheme for high-pressure physics are discussed and future improvements to the setup are suggested.

Single-shot ultrafast multiplexed coherent diffraction imaging

Classic interferometry was commonly adopted to realize ultrafast phase imaging using pulsed lasers; however, the reference beam required makes the optical structure of the imaging system very complex, and high temporal resolution was reached by sacrificing spatial resolution. This study presents a type of single-shot ultrafast multiplexed coherent diffraction imaging technique to realize ultrafast phase imaging with both high spatial and temporal resolutions using a simple optical setup, and temporal resolution of nanosecond to femtosecond scale can be realized using lasers of different pulse durations. This technique applies a multiplexed algorithm to avoid the data division in space domain or frequency domain and greatly improves the spatial resolution. The advantages of this proposed technique on both the simple optical structure and high image quality were demonstrated by imaging the generation and evaluating the laser-induced damage and accompanying phenomenon of laser filament and shock wave at a spatial resolution better than 6.96 μm and a temporal resolution better than 10 ns.

A finite difference scheme for integrating the Takagi-Taupin equations on an arbitrary orthogonal grid.

Calculating dynamical diffraction patterns for X-ray diffraction imaging techniques requires numerical integration of the Takagi-Taupin equations. This is usually performed with a simple, second-order finite difference scheme on a sheared computational grid in which two of the axes are aligned with the wavevectors of the incident and scattered beams. This dictates, especially at low scattering angles, an oblique grid of uneven step sizes. Here a finite difference scheme is presented that carries out this integration in slab-shaped samples on an arbitrary orthogonal grid by implicitly utilizing Fourier interpolation. The scheme achieves the expected second-order convergence and a similar error to the traditional approach for similarly dense grids.

High-resolution ptychographic imaging enabled by high-speed multi-pass scanning

As a coherent diffraction imaging technique, ptychography provides high-spatial resolution beyond Rayleigh's criterion of the focusing optics, but it is also sensitively affected by the decoherence coming from the spatial and temporal variations in the experiment. Here we show that high-speed ptychographic data acquisition with short exposure can effectively reduce the impact from experimental variations. To reach a cumulative dose required for a given resolution, we further demonstrate that a continuous multi-pass scan via high-speed ptychography can achieve high-resolution imaging. This low-dose scan strategy is shown to be more dose-efficient, and has potential for radiation-sensitive sample studies and time-resolved imaging.

Challenges related to tomographic reconstruction of 3D intragranular orientation fields in the presence of orientation relationships

X-ray diffraction contrast tomography (DCT) is a near-field diffraction imaging technique to characterize the 3D shape and crystallographic orientation of grains within polycrystalline samples. The presence of orientation relationships as such encountered between Σ3n annealing twins found in Cu and Ni lead to systematic diffraction spot overlap, since a significant fraction of the lattice planes is shared between the parent and twin crystal lattices. If not correctly addressed, these overlaps will lead to artifacts in the individual grain reconstruction. In this paper we introduce a strategy for joint, tomographic reconstruction of Twin Related Domains (TRD) and cost function weights into DCT to improve the grain reconstruction quality. A large-grained polycrystalline sample made from pure Ni is used for testing this approach and its ability to reveal intragranular orientation gradients related to plastic strain localization at the onset of plastic deformation in this type of materials.