Journal of Synchrotron Radiation最新文献

3D mixed perovskites have achieved substantial success in boosting solar cell efficiency, but the complicated perovskite crystal formation pathway remains mysterious. Here we present detailed crystallization kinetics of mixed perovskites FA_0.83MA_0.17Pb(I_0.83Br_0.17)₃, where FA is formamidinium and MA is methylammonium, with the addition of Cs⁺ to form a triple cation perovskite (3-CAT), in a comparison with the perovskite building block MAPbI₃ (MAPI) via static grazing-incidence wide-angle X-ray scattering (GIWAXS) and micro-diffraction measurements. Spin-coated films produced α-perovskite peaks with no PbI₂ or δ-intermediate phases, which was a promising result for the 3-CAT perovskite from micro-diffraction measurements. However, the 3-CAT did not remain stable on probing with varied relative humidity (RH) conditions as segregation back to the δ-intermediate and PbI₂ phase after 10 s of exposure to an RH value of 11% was found to occur from the GIWAXS results. When RH levels were elevated to over 100%, segregation peaks of PbI₂ and δ-intermediate (2H, 4H and 6H) became conspicuous as the α-phase intensity diminished, unlike for MAPI that remains relatively stable. The possible cause of this is hydrophilic bonds that form between the 3-CAT crystals and the small annealing window of the best composition perovskite (5% Cs⁺) film.

The performances of a spherically bent Bragg analyzer and a cylindrically bent Laue analyzer in an X-ray Raman/emission spectrometer are compared. The reflectivity and energy resolution are evaluated from the intensity of the elastic scattering and the width of the energy distribution on a SiO₂ glass sample. Widely used, Bragg analyzers display excellent performance at the photon energy E ≤ 10 keV. However, at higher E, the reflectivity and the resolution gradually deteriorate as E increases, showing poor performance above 20 keV. On the other hand, the reflectivity of the Laue analyzer gradually increases at E > 10 keV, displaying excellent reflectivity and good resolution around 20 keV. The Laue analyzer is suitable for X-ray absorption spectroscopy in high-energy-resolution fluorescence-detection mode or X-ray emission spectroscopy on 4d transition metal compounds. Furthermore, the X-ray Raman features of the lithium K-edge in LiF and the oxygen K-edge feature in H₂O, measured by nine Bragg analyzers (2 m radius) at E ≃ 9.9 keV and by five Laue analyzers (1.4 m radius) at E ≃ 19.5 keV, have been compared. Similar count rates and resolutions are observed.

We report on recent developments that enable megahertz hard X-ray phase contrast imaging (MHz XPCI) experiments at the Single Particles, Clusters, and Biomolecules and Serial Femtosecond Crystallography (SPB/SFX) instrument of the European XFEL facility (EuXFEL). We describe the technical implementation of the key components, including an MHz fast camera and a modular indirect X-ray microscope system based on fast scintillators coupled through a high-resolution optical microscope, which enable full-field X-ray microscopy with phase contrast of fast and irreversible phenomena. The image quality for MHz XPCI data showed significant improvement compared with a pilot demonstration of the technique using parallel beam illumination, which also allows access to up to 24 keV photon energies at the SPB/SFX instrument of the EuXFEL. With these developments, MHz XPCI was implemented as a new method offered for a broad user community (academic and industrial) and is accessible via standard user proposals. Furthermore, intra-train pulse diagnostics with a high few-micrometre spatial resolution and recording up to 128 images of consecutive pulses in a train at up to 1.1 MHz repetition rate is available upstream of the instrument. Together with the diagnostic camera upstream of the instrument and the MHz XPCI setup at the SPB/SFX instrument, simultaneous two-plane measurements for future beam studies and feedback for machine parameter tuning are now possible.

The combination of reversible angular dispersion-induced microbunching (ADM) and the rapid damping storage ring provides a storage-ring-based light source with the capability to produce longitudinal coherent radiation with a high repetition rate. This paper presents a prototype design for a test facility based on the study by Jiang et al. [Sci. Rep. (2022), 12, 3325]. The modulation-demodulation section is inserted into a long straight section of the storage ring instead of a bypass line, which poses great challenges for the optimization of the nonlinear dynamics of the storage ring. However, this design avoids the challenging injection and extraction system connecting to the bypass line. To utilize mature laser technology and reduce the difficulty of the reversible ADM lattice design, we use a long-wavelength 1030 nm seed laser. In the simulation, we achieved 20th harmonic radiation with a bunching factor of about 7.2%. The growth rate of vertical emittance and energy spread of the electron beam for a single pass are about 11% and 0.02%, respectively. When the energy of the electron beam is 800 MeV and two sets of damping wigglers are employed, the damping time in the vertical plane is reduced to 8.31 ms. This results in a 438 kHz repetition rate of the coherent radiation at the new equilibrium state.

One of the main limitations of conventional absorption-based X-ray micro-computed tomography imaging of biological samples is the low inherent X-ray contrast of soft tissue. To overcome this limitation, the use of ethanol as contrast agent has been proposed to enhance image contrast of soft tissues through dehydration. Some authors have shown that ethanol shrinks and hardens the tissue too much, also causing small tissue ruptures due to fast dehydration. However, the local tissue deformation occurring as a consequence of tissue dehydration and whether tissue shrinkage can modify myocardial architecture has not been quantified yet. The aim of this paper is to quantify the local myocardial tissue deformation due to ethanol dehydration based on 3D non-rigid registration and perform a detailed characterization of its myocardial tissue organization, before and after ethanol dehydration. A rat adult heart was imaged with synchrotron-radiation-based X-ray phase contrast imaging (X-PCI) three times: before, 9 h after and 342 h after ethanol immersion. The total volume shrinkage as well as changes in the left ventricular myocardial thickness were computed. Then, to determine local deformation of the heart caused by ethanol dehydration, the related 3D tomographic datasets were registered by means of a non-rigid registration algorithm. Finally, changes on the orientation and organization of myocytes were assessed. Our results show that the use of ethanol in synchrotron X-PCI can improve image contrast, but the tissue shrinkage is not homogeneous thus changing the local myocardial organization.

Coherent diffractive imaging experiments often collect incomplete datasets containing regions that lack any measurements. These regions can arise because of beamstops, gaps between detectors, or, in tomography experiments, a missing wedge of data due to a limited sample rotation range. We describe practical and effective approaches to mitigate reconstruction artifacts by bringing uniqueness back to the phase retrieval problem. This is accomplished by looking for a solution that both matches the data and has minimum total variation, which essentially sets the unconstrained modes to reduce oscillations within the reconstruction. Two algorithms are described. The first algorithm assumes that there is an accurate estimate of the phase and can be used for pre- and post-processing. The second algorithm attempts to simultaneously minimize the total variation and recover the phase. We demonstrate the utility of these algorithms with numerical simulations and, experimentally, on a large, three-dimensional dataset.

This paper introduces a novel slit-less wavelength-dispersive spectrometer design that incorporates a single-bounce monocapillary with the goal of positioning the sample directly on the Rowland circle, thereby eliminating the need for a traditional entrance slit. This configuration enhances photon throughput while preserving energy resolution, demonstrated in comparative measurements on boron nitride and different lithium nickel manganese cobalt oxide cathodes. A common alternative to an entrance slit for limiting the source size on the Rowland circle is a customized design of the beamline involving a focusing optics unit consisting of two Kirkpatrick-Baez mirrors close to the end station. The new slit-less design does not rely on specialized beamlines and can be considered, thanks to the increased efficiency, for spectrometers using laboratory based sources equipped with equivalent optics. The comparative measurements found that the resolving power achieved was E/ΔE = 1085 at 401.5 eV incident energy, and the enhancement in detection efficiency was a factor of 3.7 due to more effective utilization of the X-ray beam.

X-ray fluorescence (XRF) is widely used to analyze elemental distributions in samples. Micro-XRF (µ-XRF), the most basic conventional XRF technique, offers good spatial resolution through precise 2D scanning with a micrometre-sized X-ray source. Recently, synchrotron based XRF analysis platforms have achieved nano-XRF with highly focused X-rays using polycapillary optics or mirrors, leveraging the excellent coherence of synchrotron radiation. However, XRF techniques are hindered by long data acquisition times (exceeding several hours) due to their point-by-point scanning approach, impeding large-area elemental mapping. Full-field XRF (FF-XRF), developed in the 2010s and based on the high brilliance of synchrotron X-rays, enables significantly shorter (less than a few minutes) data acquisition times via single-exposure imaging using a 2D X-ray detector. Nevertheless, it is constrained by relatively low spatial resolution and sensitivity. Hence, a new XRF platform is required to accommodate resolution demands to cover diverse experimental purposes. In this study, we developed a preliminary model of a novel XRF system that combines micro- and full-field XRF setups to address these limitations. This system allows easy mode switching while maintaining the region of interest of the imaging system within a single apparatus, simply by rotating the sample to face either detector depending on research purposes. We anticipate that this new XRF system will be widely utilized in various research fields as the initial XRF setup at Pohang Light Source-II.

In synchrotron X-ray radiography, achieving high image resolution and an optimal signal-to-noise ratio (SNR) is crucial for the subsequent accurate image analysis. Traditional methods often struggle to balance these two parameters, especially in situ applications where rapid data acquisition is essential to capture specific dynamic processes. For quantitative image data analysis, using monochromatic X-rays is essential. A double multilayer monochromator (DMM) is successfully used for this aim at the BAMline, BESSY II (Helmholtz Zentrum Berlin, Germany). However, such DMMs are prone to producing an unstable horizontal stripe pattern. Such an unstable pattern renders proper signal normalization difficult and thereby causes a reduction of the SNR. We introduce a novel approach to enhance SNR while preserving resolution: dynamic tilting of the DMM. By adjusting the orientation of the DMM during the acquisition of radiographic projections, we optimize the X-ray imaging quality, thereby enhancing the SNR. The corresponding shift of the projection during this movement is corrected in post-processing. The latter correction allows a good resolution to be preserved. This dynamic tilting technique enables the homogenization of the beam profile and thereby effectively reduces noise while maintaining high resolution. We demonstrate that data captured using this proposed technique can be seamlessly integrated into the existing radiographic data workflow, as it does not need hardware modifications to classical X-ray imaging beamline setups. This facilitates further image analysis and processing using established methods.

Geological samples are inherently multi-scale. Understanding their bulk physical and chemical properties requires characterization down to the nano-scale. A powerful technique to study the three-dimensional microstructure is X-ray tomography, but it lacks information about the chemistry of samples. To develop a methodology for measuring the multi-scale 3D microstructure of geological samples, correlative X-ray micro- and nanotomography were performed on two rocks followed by scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS) analysis. The study was performed in five steps: (i) micro X-ray tomography was performed on rock sample cores, (ii) samples for nanotomography were prepared using laser milling, (iii) nanotomography was performed on the milled sub-samples, (iv) samples were mounted and polished for SEM analysis and (v) SEM imaging and compositional mapping was performed on micro and nanotomography samples for complimentary information. Correlative study performed on samples of serpentine and basalt revealed multiscale 3D structures involving both solid mineral phases and pore networks. Significant differences in the volume fraction of pores and mineral phases were also observed dependent on the imaging spatial resolution employed. This highlights the necessity for the application of such a multiscale approach for the characterization of complex aggregates such as rocks. Information acquired from the chemical mapping of different phases was also helpful in segmentation of phases that did not exhibit significant contrast in X-ray imaging. Adoption of the protocol used in this study can be broadly applied to 3D imaging studies being performed at the Advanced Light Source and other user facilities.