IDATEN and G‐SITENNO: GUI‐assisted software for coherent X‐ray diffraction imaging experiments and data analyses at SACLA

Using our custom‐made diffraction apparatus KOTOBUKI‐1 and two multiport CCD detectors, cryogenic coherent X‐ray diffraction imaging experiments have been undertaken at the SPring‐8 Angstrom Compact free electron LAser (SACLA) facility. To efficiently perform experiments and data processing, two software suites with user‐friendly graphical user interfaces have been developed. The first is a program suite named IDATEN, which was developed to easily conduct four procedures during experiments: aligning KOTOBUKI‐1, loading a flash‐cooled sample into the cryogenic goniometer stage inside the vacuum chamber of KOTOBUKI‐1, adjusting the sample position with respect to the X‐ray beam using a pair of telescopes, and collecting diffraction data by raster scanning the sample with X‐ray pulses. Named G‐SITENNO, the other suite is an automated version of the original SITENNO suite, which was designed for processing diffraction data. These user‐friendly software suites are now indispensable for collecting a large number of diffraction patterns and for processing the diffraction patterns immediately after collecting data within a limited beam time.     

A feasibility study of dynamic stress analysis inside a running internal combustion engine using synchrotron X‐ray beams

The present investigation establishes the feasibility of using synchrotron‐generated X‐ray beams for time‐resolved in situ imaging and diffraction of the interior components of an internal combustion engine during its operation. The demonstration experiment was carried out on beamline I12 (JEEP) at Diamond Light Source, UK. The external hutch of the JEEP instrument is a large‐scale engineering test bed for complex in situ processing and simulation experiments. The hutch incorporates a large capacity translation and rotation table and a selection of detectors for monochromatic and white‐beam diffraction and imaging. These capabilities were used to record X‐ray movies of a motorcycle internal combustion engine running at 1850 r.p.m. and to measure strain inside the connecting rod via stroboscopic X‐ray diffraction measurement. The high penetrating ability and high flux of the X‐ray beam at JEEP allowed the observation of inlet and outlet valve motion, as well as that of the piston, connecting rod and the timing chain within the engine. Finally, the dynamic internal strain within the moving connecting rod was evaluated with an accuracy of ～50 × 10^?6.     

Individual GaAs nanorods imaged by coherent X‐ray diffraction

Using scanning X‐ray diffraction microscopy with a spot size of 220 × 600 nm, it was possible to inspect individual GaAs nanorods grown seed‐free through circular openings in a SiN_x mask in a periodic array with 3 µm spacing on GaAs[111]B. The focused X‐ray beam allows the determination of the strain state of individual rods and, in combination with coherent diffraction imaging, it was also possible to characterize morphological details. Rods grown either in the centre or at the edge of the array show significant differences in shape, size and strain state.     

Development of variable‐magnification X‐ray Bragg optics

A novel X‐ray Bragg optics is proposed for variable‐magnification of an X‐ray beam. This X‐ray Bragg optics is composed of two magnifiers in a crossed arrangement, and the magnification factor, M, is controlled through the azimuth angle of each magnifier. The basic properties of the X‐ray optics such as the magnification factor, image transformation matrix and intrinsic acceptance angle are described based on the dynamical theory of X‐ray diffraction. The feasibility of the variable‐magnification X‐ray Bragg optics was verified at the vertical‐wiggler beamline BL‐14B of the Photon Factory. For X‐ray Bragg magnifiers, Si(220) crystals with an asymmetric angle of 14° were used. The magnification factor was calculated to be tunable between 0.1 and 10.0 at a wavelength of 0.112 nm. At various magnification factors (M≥ 1.0), X‐ray images of a nylon mesh were observed with an air‐cooled X‐ray CCD camera. Image deformation caused by the optics could be corrected by using a 2 × 2 transformation matrix and bilinear interpolation method. Not only absorption‐contrast but also edge‐contrast due to Fresnel diffraction was observed in the magnified images.     

Focusing femtosecond X‐ray free‐electron laser pulses by refractive lenses

The possibility of using a parabolic refractive lens with initial X‐ray free‐electron laser (XFEL) pulses, i.e. without a monochromator, is analysed. It is assumed that the measurement time is longer than 0.3 fs, which is the time duration of a coherent pulse (spike). In this case one has to calculate the propagation of a monochromatic wave and then perform an integration of the intensity over the radiation spectrum. Here a general algorithm for calculating the propagation of time‐dependent radiation in free space and through various objects is presented. Analytical formulae are derived describing the properties of the monochromatic beam focused by a system of one and two lenses. Computer simulations show that the European XFEL pulses can be focused with maximal efficiency, i.e. as for a monochromatic wave. This occurs even for nanofocusing lenses.     

X‐ray focusing by the system of refractive lens(es) placed inside asymmetric channel‐cut crystals

An X‐ray one‐dimensionally focusing system, a refracting–diffracting lens (RDL), composed of Bragg double‐asymmetric‐reflecting two‐crystal plane parallel plates and a double‐concave cylindrical parabolic lens placed in the gap between the plates is described. It is shown that the focal length of the RDL is equal to the focal distance of the separate lens multiplied by the square of the asymmetry factor. One can obtain RDLs with different focal lengths for certain applications. Using the point‐source function of dynamic diffraction, as well as the Green function in a vacuum with parabolic approximation, an expression for the double‐diffracted beam amplitude for an arbitrary incident wave is presented. Focusing of the plane incident wave and imaging of a point source are studied. The cases of non‐absorptive and absorptive lenses are discussed. The intensity distribution in the focusing plane and on the focusing line, and its dependence on wavelength, deviation from the Bragg angle and magnification is studied. Geometrical optical considerations are also given. RDLs can be applied to focus radiation from both laboratory and synchrotron X‐ray sources, for X‐ray imaging of objects, and for obtaining high‐intensity beams. RDLs can also be applied in X‐ray astronomy.     

Application of a pnCCD in X‐ray diffraction: a three‐dimensional X‐ray detector

The first application of a pnCCD detector for X‐ray scattering experiments using white synchrotron radiation at BESSY II is presented. A Cd arachidate multilayer was investigated in reflection geometry within the energy range 7 keV < E < 35 keV. At fixed angle of incidence the two‐dimensional diffraction pattern containing several multilayer Bragg peaks and respective diffuse‐resonant Bragg sheets were observed. Since every pixel of the detector is able to determine the energy of every incoming photon with a resolution ΔE/E? 10^?2, a three‐dimensional dataset is finally obtained. In order to achieve this energy resolution the detector was operated in the so‐called single‐photon‐counting mode. A full dataset was evaluated taking into account all photons recorded within 10⁵ detector frames at a readout rate of 200 Hz. By representing the data in reciprocal‐space coordinates, it becomes obvious that this experiment with the pnCCD detector provides the same information as that obtained by combining a large number of monochromatic scattering experiments using conventional area detectors.     

High‐energy transmission Laue micro‐beam X‐ray diffraction: a probe for intra‐granular lattice orientation and elastic strain in thicker samples

An understanding of the mechanical response of modern engineering alloys to complex loading conditions is essential for the design of load‐bearing components in high‐performance safety‐critical aerospace applications. A detailed knowledge of how material behaviour is modified by fatigue and the ability to predict failure reliably are vital for enhanced component performance. Unlike macroscopic bulk properties (e.g. stiffness, yield stress, etc.) that depend on the average behaviour of many grains, material failure is governed by `weakest link'‐type mechanisms. It is strongly dependent on the anisotropic single‐crystal elastic–plastic behaviour, local morphology and microstructure, and grain‐to‐grain interactions. For the development and validation of models that capture these complex phenomena, the ability to probe deformation behaviour at the micro‐scale is key. The diffraction of highly penetrating synchrotron X‐rays is well suited to this purpose and micro‐beam Laue diffraction is a particularly powerful tool that has emerged in recent years. Typically it uses photon energies of 5–25 keV, limiting penetration into the material, so that only thin samples or near‐surface regions can be studied. In this paper the development of high‐energy transmission Laue (HETL) micro‐beam X‐ray diffraction is described, extending the micro‐beam Laue technique to significantly higher photon energies (50–150 keV). It allows the probing of thicker sample sections, with the potential for grain‐level characterization of real engineering components. The new HETL technique is used to study the deformation behaviour of individual grains in a large‐grained polycrystalline nickel sample during in situ tensile loading. Refinement of the Laue diffraction patterns yields lattice orientations and qualitative information about elastic strains. After deformation, bands of high lattice misorientation can be identified in the sample. Orientation spread within individual scattering volumes is studied using a pattern‐matching approach. The results highlight the inability of a simple Schmid‐factor model to capture the behaviour of individual grains and illustrate the need for complementary mechanical modelling.     

Fabrication and testing of a newly designed slit system for depth‐resolved X‐ray diffraction measurements

A new system of slits called `spiderweb slits' have been developed for depth‐resolved powder or polycrystalline X‐ray diffraction measurements. The slits act on diffracted X‐rays to select a particular gauge volume of sample, while absorbing diffracted X‐rays from outside of this volume. Although the slit geometry is to some extent similar to that of previously developed conical slits or spiral slits, this new design has advantages over the previous ones in use for complex heterogeneous materials and in situ and operando diffraction measurements. For example, the slits can measure a majority of any diffraction cone for any polycrystalline material, over a continuous range of diffraction angles, and work for X‐ray energies of tens to hundreds of kiloelectronvolts. The design is generated and optimized using ray‐tracing simulations, and fabricated through laser micromachining. The first prototype was successfully tested at the X17A beamline at the National Synchrotron Light Source, and shows similar performance to simulations, demonstrating gauge volume selection for standard powders, for all diffraction peaks over angles of 2–10°. A similar, but improved, design will be implemented at the X‐ray Powder Diffraction beamline at the National Synchrotron Light Source II.     

White‐beam X‐ray radioscopy and tomography with simultaneous diffraction at the EDDI beamline

A set‐up for simultaneous imaging and diffraction that yields radiograms with up to 200 frames per second and 5.6 µm effective pixel size is presented. Tomograms and diffractograms are acquired together in 10 s. Two examples illustrate the attractiveness of combining these methods at the EDDI beamline for in situ studies.     

Diffraction theory applied to X‐ray imaging with clessidra prism array lenses

Clessidra (hourglass) lenses, i.e. two large prisms each composed of smaller identical prisms or prism‐like objects, can focus X‐rays. As these lenses have a periodic structure perpendicular to the incident radiation, they will diffract the beam like a diffraction grating. Refraction in the prisms is responsible for blazing, i.e. for the concentration of the diffracted intensity into only a few diffraction peaks. It is found that the diffraction of coherent radiation in clessidra lenses needs to be treated in the Fresnel, or near‐field, regime. Here, diffraction theory is applied appropriately to the clessidra structure in order to show that blazing in a perfect structure with partly curved prisms can indeed concentrate the diffracted intensity into only one peak. When the lens is entirely composed of identical perfect prisms, small secondary peaks are found. Nevertheless, the loss in intensity in the central peak will not lead to any significant widening of this peak. Clessidras with perfect prisms illuminated by full coherent X‐ray radiation can then provide spatial resolutions, which are consistent with the increased aperture, and which are far below the height of the single small prisms.     

Coherent X‐ray scattering beamline at port 9C of Pohang Light Source II

The coherent X‐ray scattering beamline at the 9C port of the upgraded Pohang Light Source (PLS‐II) at Pohang Accelerator Laboratory in Korea is introduced. This beamline provides X‐rays of 5–20 keV, and targets coherent X‐ray experiments such as coherent diffraction imaging and X‐ray photon correlation spectroscopy. The main parameters of the beamline are summarized, and some preliminary experimental results are described.     

X‐ray photon correlation spectroscopy in systems without long‐range order: existence of an intermediate‐field regime

Successful X‐ray photon correlation spectroscopy studies often require that signals be optimized while minimizing power density in the sample to decrease radiation damage and, at free‐electron laser sources, thermal impact. This suggests exploration of scattering outside the Fraunhofer far‐field diffraction limit d²/λR, where d is the incident beam size, λ is the photon wavelength and R is the sample‐to‐detector distance. Here it is shown that, in an intermediate regime d²/λ > Rdξ/λ, where ξ is the structural correlation length in the material, the ensemble averages of the scattered intensity and of the structure factor are equal. Similarly, in the regime d²/λ > Rdξ(τ)/λ, where ξ(τ) is a time‐dependent dynamics length scale of interest, the ensemble‐averaged correlation functions g₁(τ) and g₂(τ) of the scattered electric field are also equal to their values in the far‐field limit. This broadens the parameter space for X‐ray photon correlation spectroscopy experiments, but detectors with smaller pixel size and variable focusing are required to more fully exploit the potential for such studies.     

In situ X‐ray diffraction study on the growth kinetics of NiO nanoparticles

The growth kinetics of NiO nanoparticles have been studied by in situ X‐ray diffraction using two detection systems (conventional and imaging plate). NiO nanoparticles were formed by thermal decomposition after heating of an amorphous compound formed by the coprecipitation method. It was found that the detection method using an imaging plate is more efficient than the conventional detection mode for observing changes in the crystallite growth of nanocrystalline materials. Studies have been carried out to investigate the effects of the heating rates on the particles growth. The results suggest that the growth process of the particles is accelerated when the samples are treated at low heating rates. The evolution of particles size and the diffusion coefficient obtained from X‐ray powder diffraction patterns are discussed in terms of the thermal conditions for the two types of detection.     

Full‐field X‐ray reflection microscopy of epitaxial thin‐films

Novel X‐ray imaging of structural domains in a ferroelectric epitaxial thin film using diffraction contrast is presented. The full‐field hard X‐ray microscope uses the surface scattering signal, in a reflectivity or diffraction experiment, to spatially resolve the local structure with 70 nm lateral spatial resolution and sub‐nanometer height sensitivity. Sub‐second X‐ray exposures can be used to acquire a 14 µm × 14 µm image with an effective pixel size of 20 nm on the sample. The optical configuration and various engineering considerations that are necessary to achieve optimal imaging resolution and contrast in this type of microscopy are discussed.     

Novel silica stabilization method for the analysis of fine nanocrystals using coherent X‐ray diffraction imaging

High‐energy X‐ray Bragg coherent diffraction imaging (BCDI) is a well established synchrotron‐based technique used to quantitatively reconstruct the three‐dimensional morphology and strain distribution in nanocrystals. The BCDI technique has become a powerful analytical tool for quantitative investigations of nanocrystals, nanotubes, nanorods and more recently biological systems. BCDI has however typically failed for fine nanocrystals in sub‐100 nm size regimes – a size routinely achievable by chemical synthesis – despite the spatial resolution of the BCDI technique being 20–30 nm. The limitations of this technique arise from the movement of nanocrystals under illumination by the highly coherent beam, which prevents full diffraction data sets from being acquired. A solution is provided here to overcome this problem and extend the size limit of the BCDI technique, through the design of a novel stabilization method by embedding the fine nanocrystals into a silica matrix. Chemically synthesized FePt nanocrystals of maximum dimension 20 nm and AuPd nanocrystals in the size range 60–65 nm were investigated with BCDI measurement at beamline 34‐ID‐C of the APS, Argonne National Laboratory. Novel experimental methodologies to elucidate the presence of strain in fine nanocrystals are a necessary pre‐requisite in order to better understand strain profiles in engineered nanocrystals for novel device development.     

Quick X‐ray reflectivity using monochromatic synchrotron radiation for time‐resolved applications

A new technique for the parallel collection of X‐ray reflectivity (XRR) data, compatible with monochromatic synchrotron radiation and flat substrates, is described and applied to the in situ observation of thin‐film growth. The method employs a polycapillary X‐ray optic to produce a converging fan of radiation, incident onto a sample surface, and an area detector to simultaneously collect the XRR signal over an angular range matching that of the incident fan. Factors determining the range and instrumental resolution of the technique in reciprocal space, in addition to the signal‐to‐background ratio, are described in detail. This particular implementation records ～5° in 2gθ and resolves Kiessig fringes from samples with layer thicknesses ranging from 3 to 76 nm. The value of this approach is illustrated by showing in situ XRR data obtained with 100 ms time resolution during the growth of epitaxial La_0.7Sr_0.3MnO₃ on SrTiO₃ by pulsed laser deposition at the Cornell High Energy Synchrotron Source (CHESS). Compared with prior methods for parallel XRR data collection, this is the first method that is both sample‐independent and compatible with the highly collimated, monochromatic radiation typical of third‐generation synchrotron sources. Further, this technique can be readily adapted for use with laboratory‐based sources.     

Confocal full‐field X‐ray microscope for novel three‐dimensional X‐ray imaging

A confocal full‐field X‐ray microscope has been developed for use as a novel three‐dimensional X‐ray imaging method. The system consists of an X‐ray illuminating `sheet‐beam' whose beam shape is micrified only in one dimension, and an X‐ray full‐field microscope whose optical axis is normal to the illuminating sheet beam. An arbitral cross‐sectional region of the object is irradiated by the sheet‐beam, and secondary X‐ray emission such as fluorescent X‐rays from this region is imaged simultaneously using the full‐field microscope. This system enables a virtual sliced image of a specimen to be obtained as a two‐dimensional magnified image, and three‐dimensional observation is available only by a linear translation of the object along the optical axis of the full‐field microscope. A feasibility test has been carried out at beamline 37XU of SPring‐8. Observation of the three‐dimensional distribution of metallic inclusions in an artificial diamond was performed.     

Diffractive–refractive optics: X‐ray splitter

The possibility of splitting a thin (e.g. undulator) X‐ray beam based on diffraction–refraction effects is discussed. The beam is diffracted from a crystal whose diffracting surface has the shape of a roof with the ridge lying in the plane of diffraction. The crystal is cut asymmetrically. One half of the beam impinges on the left‐hand part of the roof and the other half impinges on the right‐hand side of the roof. Owing to refraction the left part of the beam is deviated to the left whereas the right part is deviated to the right. The device proposed consists of two channel‐cut crystals with roof‐like diffraction surfaces; the crystals are set in a dispersive position. The separation of the beams after splitting is calculated at a distance of 10 m from the crystals for various asymmetry and inclination angles. It is shown that such a splitting may be utilized for long beamlines. Advantages and disadvantages of this method are discussed.     

Spectrometer for hard X‐ray free‐electron laser based on diffraction focusing

X‐ray free‐electron lasers (XFELs) generate sequences of ultra‐short spatially coherent pulses of X‐ray radiation. A diffraction focusing spectrometer (DFS), which is able to measure the whole energy spectrum of the radiation of a single XFEL pulse with an energy resolution of ΔE/E? 2 × 10^?6, is proposed. This is much better than for most modern X‐ray spectrometers. Such resolution allows one to resolve the fine spectral structure of the XFEL pulse. The effect of diffraction focusing occurs in a single‐crystal plate due to dynamical scattering, and is similar to focusing in a Pendry lens made from a metamaterial with a negative refraction index. Such a spectrometer is easier to operate than those based on bent crystals. It is shown that the DFS can be used in a wide energy range from 5 keV to 20 keV.