Automatic marker-based alignment method for a nano-resolution full-field transmission X-ray microscope.

Driven by the development of X-ray optics, the spatial resolution of the full-field transmission X-ray microscope (TXM) has reached tens of nanometers and plays an important role in promoting the development of biomedicine and materials science. However, due to the thermal drift and the radial/axial motion error of the rotation stage, TXM computed tomography (CT) data are often associated with random image jitter errors along the horizontal and vertical directions during CT measurement. A nano-resolution 3D structure information reconstruction is almost impossible without a prior appropriate alignment process. To solve this problem, a fully automatic gold particle marker-based alignment approach without human intervention was proposed in this study. It can automatically detect, isolate, and register gold particles for projection image alignment with high efficiency and accuracy, facilitating a high-quality tomographic reconstruction. Simulated and experimental results confirmed the reliability and robustness of this method.

Stereoselective coronas regulate the fate of chiral gold nanoparticles in vivo.

It is unknown how the identity provided by protein coronas on the surface of chiral nanoparticles determines their blood circulation, distribution, and clearance fates of the nanoparticles in vivo. Here, we attempt to investigate how the mirrored surface of gold nanoparticles with distinct chirality reshapes the coronal composition that mediates their subsequent clearance from blood and biodistribution. We found that chiral gold nanoparticles exhibited surface chirality-specific recognition for the coronal components, including the lipoproteins, complement components, and acute phase proteins, ultimately resulting in distinct cell uptake and tissue accumulation in vivo. We observed that these stereoselective behaviors were correlated to subgroups of the corona composition that could bind to low-density lipoprotein receptors. Therefore, this study reveals how chirality-specific protein compositions selectively recognize and interact with cell receptors for chirality-mediated tissue accumulation. This study will deepen our understanding of how chiral nanoparticles/nanomedicine/nanocarriers interact with biological systems to guide the efficient fabrication of target nanomedicines.

Deep-learning-based ring artifact correction for tomographic reconstruction.

X-ray tomography has been widely used in various research fields thanks to its capability of observing 3D structures with high resolution non-destructively. However, due to the nonlinearity and inconsistency of detector pixels, ring artifacts usually appear in tomographic reconstruction, which may compromise image quality and cause nonuniform bias. This study proposes a new ring artifact correction method based on the residual neural network (ResNet) for X-ray tomography. The artifact correction network uses complementary information of each wavelet coefficient and a residual mechanism of the residual block to obtain high-precision artifacts through low operation costs. In addition, a regularization term is used to accurately extract stripe artifacts in sinograms, so that the network can better preserve image details while accurately separating artifacts. When applied to simulation and experimental data, the proposed method shows a good suppression of ring artifacts. To solve the problem of insufficient training data, ResNet is trained through the transfer learning strategy, which brings advantages of robustness, versatility and low computing cost.

A magnetically controlled chemical-mechanical polishing (MC-CMP) approach for fabricating channel-cut silicon crystal optics for the High Energy Photon Source.

Crystal monochromators are indispensable optical components for the majority of beamlines at synchrotron radiation facilities. Channel-cut monochromators are sometimes chosen to filter monochromatic X-ray beams by virtue of their ultrahigh angular stability. Nevertheless, high-accuracy polishing on the inner diffracting surfaces remains challenging, thus hampering their performance in preserving the coherence or wavefront of the photon beam. Herein, a magnetically controlled chemical-mechanical polishing (MC-CMP) approach has been successfully developed for fine polishing of the inner surfaces of channel-cut crystals. This MC-CMP process relieves the constraints of narrow working space dictated by small offset requirements and achieves near-perfect polishing on the surface of the crystals. Using this method, a high-quality surface with roughness of 0.614 nm (root mean square, r.m.s.) is obtained in a channel-cut crystal with 7 mm gap designed for beamlines at the High Energy Photon Source, a fourth-generation synchrotron radiation source under construction. On-line X-ray topography and rocking-curve measurements indicate that the stress residual layer on the crystal surface was removed. Firstly, the measured rocking-curve width is in good agreement with the theoretical value. Secondly, the peak reflectivity is very close to theoretical values. Thirdly, topographic images of the optics after polishing were uniform without any speckle or scratches. Only a nearly 2.5 nm-thick SiO2 layer was observed on the perfect crystalline matrix from high-resolution transmission electron microscopy photographs, indicating that the structure of the bulk material is defect- and dislocation-free. Future development of MC-CMP is promising for fabricating wavefront-preserving and ultra-stable channel-cut monochromators, which are crucial to exploit the merits of fourth-generation synchrotron radiation sources or hard X-ray free-electron lasers.

Feature detection network-based correction method for accurate nano-tomography reconstruction.

Driven by the development of advanced x-ray optics such as Fresnel zone plates, nano-resolution full-field transmission x-ray microscopy (Nano-CT) has become a powerful technique for the non-destructive volumetric inspection of objects and has long been developed at different synchrotron radiation facilities. However, Nano-CT data are often associated with random sample jitter because of the drift or radial/axial error motion of the rotation stage during measurement. Without a proper sample jitter correction process prior to reconstruction, the use of Nano-CT in providing accurate 3D structure information for samples is almost impossible. In this paper, to realize accurate 3D reconstruction for Nano-CT, a correction method based on a feature detection neural network, which can automatically extract target features from a projective image and precisely correct sample jitter errors, is proposed, thereby resulting in high-quality nanoscale 3D reconstruction. Compared with other feature detection methods, even if the target feature is overlapped by other high-density materials or impurities, the proposed Nano-CT correction method still acquires sub-pixel accuracy in geometrical correction and is more suitable for Nano-CT reconstruction because of its universal and faster correction speed. The simulated and experimental datasets demonstrated the reliability and validity of the proposed Nano-CT correction method.

Inhibiting weld cracking in high-strength aluminium alloys.

Cracking from a fine equiaxed zone (FQZ), often just tens of microns across, plagues the welding of 7000 series aluminum alloys. Using a multiscale correlative methodology, from the millimeter scale to the nanoscale, we shed light on the strengthening mechanisms and the resulting intergranular failure at the FQZ. We show that intergranular AlCuMg phases give rise to cracking by micro-void nucleation and subsequent link-up due to the plastic incompatibility between the hard phases and soft (low precipitate density) grain interiors in the FQZ. To mitigate this, we propose a hybrid welding strategy exploiting laser beam oscillation and a pulsed magnetic field. This achieves a wavy and interrupted FQZ along with a higher precipitate density, thereby considerably increasing tensile strength over conventionally hybrid welded butt joints, and even friction stir welds.

Deep-learning-based image registration for nano-resolution tomographic reconstruction.

Nano-resolution full-field transmission X-ray microscopy has been successfully applied to a wide range of research fields thanks to its capability of non-destructively reconstructing the 3D structure with high resolution. Due to constraints in the practical implementations, the nano-tomography data is often associated with a random image jitter, resulting from imperfections in the hardware setup. Without a proper image registration process prior to the reconstruction, the quality of the result will be compromised. Here a deep-learning-based image jitter correction method is presented, which registers the projective images with high efficiency and accuracy, facilitating a high-quality tomographic reconstruction. This development is demonstrated and validated using synthetic and experimental datasets. The method is effective and readily applicable to a broad range of applications. Together with this paper, the source code is published and adoptions and improvements from our colleagues in this field are welcomed.

Automatic 3D image registration for nano-resolution chemical mapping using synchrotron spectro-tomography.

Nano-resolution synchrotron X-ray spectro-tomography has been demonstrated as a powerful tool for probing the three-dimensional (3D) structural and chemical heterogeneity of a sample. By reconstructing a number of tomographic data sets recorded at different X-ray energy levels, the energy-dependent intensity variation in every given voxel fingerprints the corresponding local chemistry. The resolution and accuracy of this method, however, could be jeopardized by non-ideal experimental conditions, e.g. instability in the hardware system and/or in the sample itself. Herein is presented one such case, in which unanticipated sample deformation severely degrades the data quality. To address this issue, an automatic 3D image registration method is implemented to evaluate and correct this effect. The method allows the redox heterogeneity in partially delithiated LixTa0.3Mn0.4O2 battery cathode particles to be revealed with significantly improved fidelity.

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide.

Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li1.2Ni0.13Mn0.54Co0.13O2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles' core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.

Multi-contrast diffraction enhanced computed laminography at Beijing Synchrotron Radiation Facility.

Synchrotron radiation X-ray computed tomography (CT) enables nondestructive visualization of 3D morphological and chemical changes inside a sample and has become a powerful analysis tool to monitor reactive parts and their chemical states. However, synchrotron radiation CT imaging of specimens with lateral extensions much larger than the acceptance window of detectors is rather problematic due to strong absorption of X-rays in the lateral directions. On the other hand, X-ray computed laminography (CL) permits 3D imaging of flat samples while X-ray diffraction enhanced imaging (DEI) can provide high-quality results with different imaging contrasts such as absorption, phase and dark-field for samples with weak absorptions. Combining CL and DEI together, we have developed a multi-contrast DEI-CL system at the 4W1A beamline of the Beijing Synchrotron Radiation Facility for this kind of sample. Here we reported its design, implementation, and preliminary experimental results of carbon fiber reinforced polymer laminates with three kinds of imaging contrasts. The results have demonstrated the validity of this DEI-CL system. It will be helpful to push the applications of the state-of-the-art synchrotron radiation methods and instruments towards cutting-edge research. Graphical abstract ᅟ.

Absorption, refraction and scattering retrieval in X-ray analyzer-based imaging.

A three-image algorithm is proposed in order to retrieve the absorption, refraction and ultra-small-angle X-ray scattering (USAXS) properties of the object in X-ray analyzer-based imaging. Based on the Gaussian fitting to the rocking curve, the novel algorithm is theoretically derived and presented, and validated by synchrotron radiation experiments. Compared with multiple-image radiography, this algorithm only requires a minimum of three intensity measurements, and is therefore advantageous in terms of simplified acquisition procedure and reduced data collection times, which are especially important for specific applications such as in vivo imaging and phase tomography. Moreover, the retrieval algorithm can be specialized to particular cases where some degree of a priori knowledge on the object is available, potentially reducing the minimum number of intensity measurements to two. Furthermore, the effect of angular mis-alignment on the accuracy of the retrieved images was theoretically investigated, which can be of use in image interpretation and optimization of the data acquisition procedure.

Propagation topography of redox phase transformations in heterogeneous layered oxide cathode materials.

Redox phase transformations are relevant to a number of metrics pertaining to the electrochemical performance of batteries. These phase transformations deviate from and are more complicated than the conventional theory of phase nucleation and propagation, owing to simultaneous changes of cationic and anionic valence states as well as the polycrystalline nature of battery materials. Herein, we propose an integrative approach of mapping valence states and constructing chemical topographies to investigate the redox phase transformation in polycrystalline layered oxide cathode materials under thermal abuse conditions. We discover that, in addition to the three-dimensional heterogeneous phase transformation, there is a mesoscale evolution of local valence curvatures in valence state topographies. The relative probability of negative and positive local valence curvatures alternates during the layered-to-spinel/rocksalt phase transformation. The implementation of our method can potentially provide a universal approach to study phase transformation behaviors in battery materials and beyond.

Angular signal radiography.

Microscopy techniques using visible photons, x-rays, neutrons, and electrons have made remarkable impact in many scientific disciplines. The microscopic data can often be expressed as the convolution of the spatial distribution of certain properties of the specimens and the inherent response function of the imaging system. The x-ray grating interferometer (XGI), which is sensitive to the deviation angle of the incoming x-rays, has attracted significant attention in the past years due to its capability in achieving x-ray phase contrast imaging with low brilliance source. However, the comprehensive and analytical theoretical framework is yet to be presented. Herein, we propose a theoretical framework termed angular signal radiography (ASR) to describe the imaging process of the XGI system in a classical, comprehensive and analytical manner. We demonstrated, by means of theoretical deduction and synchrotron based experiments, that the spatial distribution of specimens' physical properties, including absorption, refraction and scattering, can be extracted by ASR in XGI. Implementation of ASR in XGI offers advantages such as simplified phase retrieval algorithm, reduced overall radiation dose, and improved image acquisition speed. These advantages, as well as the limitations of the proposed method, are systematically investigated in this paper.

A Preliminary Study on Sinus Fungus Ball with MicroCT and X-Ray Fluorescence Technique.

BACKGROUND: Sinus fungus ball, an accumulation of fungal dense concretions, is a common disease in practice, and might cause fatal complications or lead to death once converted into invasive type. Early preoperative diagnosis of this disease can lead to appropriate treatment for patients and prevent multiple surgical procedures. Up to now, the diagnostic criteria of sinus fungus ball have been defined and computed tomography (CT) scan was considered as a valuable preoperative diagnostic tool. However, the sensitivity of clinical CT is only about 62%. Thus, investigating the factors which influence sensitivity is necessary for clinical CT to be a more valuable preoperative diagnosis tool. Furthermore, CT scan usually presents micro-calcifications or spots with metallic density in sinus fungus ball. Previous literatures show that there are some metallic elements such as calcium and zinc in fungus ball, and they concluded that endodontic treatment has a strong correlation with the development of maxillary sinus fungus ball and zinc ion was an exogenous risk factor. But the pathogenesis of sinus fungus ball still remains unclear because fungus ball can also develop in other non-maxillary sinuses or the maxillary sinus without root canal treatment. Is zinc ion the endogenous factor? Study on this point might be also helpful for investigating the pathogenesis of sinus fungus ball. In this paper, we tried to investigate the factors which influence the sensitivity of clinical CT by imaging sinus fungus ball with microCT. The origin of zinc ion was also studied through elements test for different fungal ball samples using x-ray fluorescence technique. METHODS: Specimens including fungal ball material and sinus mucosa from patients confirmed by pathological findings were extracted after surgery. All fungal ball specimens came from sphenoid sinus, ethmoidal sinus and maxillary sinus with or without previous endodontic treatment respectively. All of them were imaged by microCT with spatial resolution up to 5µm to acquire three-dimensional structure, and then the heavy metal elements were detected with x-ray fluorescence spectrometer analysis. RESULT: High concentration of zinc and calcium were detected in all fungal ball specimens compared to sinus mucosa membrane. Particles with different size varied from disperse to density, which have similar shape to the result of clinical CT but with different size, were found in three-dimensional reconstruction results of microCT. CONCLUSIONS: Spatial resolution is an influent factor of clinical CT sensitivity for sinus fungus ball. Improving the resolution of clinical CT will help to improve its sensitivity. Besides iatrogenic endodontic materials, endogenous metal elements of zinc and calcium might associate with the growth of fungal ball and the micro-calcifications or spots with metallic density of CT imaging.

Sub-500 nm hard x ray focusing by compound long kinoform lenses.

The focusing performance of polymethyl methacrylate compound long kinoform lenses with 70 µm aperture and 19.5 mm focal length was characterized with 8 keV x rays using the knife-edge scan method at the 4W1A transmission x-ray microscope beamline of Beijing Synchrotron Radiation Facility. The experiment result shows a best FWHM focus size of 440 nm with 31% diffraction efficiency.

Nondestructive estimation of growth year in ginseng cultivars using the means of mathematical modeling on the basis of allometry.

Growth-year authentication has extraordinary significance for plant growth, structure and development research, and has a wide range of applications in value assessment of economic crops. Panax ginseng is the most commonly used medicinal plant in Asian countries. The fix number of growth-year is an important quality evaluation which is difficult to be obtained accurately in current technical conditions. Preliminary authentication theory for growth-year has been described in previous studies using a short-lived perennial medicinal plant (Paeonia lactiflora pall.) as the research material. In this research, we focused on the growth-year estimation in ginseng cultivars, and attempt to explore the age estimation method for vascular plants according to mathematical simulation of the root structure development. Micro data was obtained from 204 individuals of 3 different kinds of ginseng cultivars, which have a series of gradient age and a clear growth record. Outer diameter of the vascular cambium (b) and the radius of cross section (r) were measured with ordinary stereo microscope. We further designed and established two different kinds of authentication model based on the taproot structure development for growth year authentication (P =ß*M-α and M = K*X1 (a) (1) X2 (a) (2) ). Moreover, the models were applied to identify the growth year of ginseng without damage using Micro-CT or DEI reconstruction. A potential method, have been recently described, the age of ginseng can be analyzed by telomere length and telomerase activity. However, we found that there are different results indicated in other species. We concluded that microscopic methods perceived currently were provided a more effective means for growth-year authentication.

A novel crystal-analyzer phase retrieval algorithm and its noise property.

A description of the rocking curve in diffraction enhanced imaging (DEI) is presented in terms of the angular signal response function and a simple multi-information retrieval algorithm based on the cosine function fitting. A comprehensive analysis of noise properties of DEI is also given considering the noise transfer characteristic of the X-ray source. The validation has been performed with synchrotron radiation experimental data and Monte Carlo simulations based on the Geant4 toolkit combined with the refractive process of X-rays, which show good agreement with each other. Moreover, results indicate that the signal-to-noise ratios of the refraction and scattering images are about one order of magnitude better than that of the absorption image at the edges of low-Z samples. The noise penalty is drastically reduced with the increasing photon flux and visibility. Finally, this work demonstrates that the analytical method can build an interesting connection between DEI and GDPCI (grating-based differential phase contrast imaging) and is widely suitable for a variety of measurement noise in the angular signal response imaging prototype. The analysis significantly contributes to the understanding of noise characteristics of DEI images and may allow improvements to the signal-to-noise ratio in biomedical and material science imaging.

Use of Synchrotron Radiation-Analytical Techniques To Reveal Chemical Origin of Silver-Nanoparticle Cytotoxicity.

To predict potential medical value or toxicity of nanoparticles (NPs), it is necessary to understand the chemical transformation during intracellular processes of NPs. However, it is a grand challenge to capture a high-resolution image of metallic NPs in a single cell and the chemical information on intracellular NPs. Here, by integrating synchrotron radiation-beam transmission X-ray microscopy (SR-TXM) and SR-X-ray absorption near edge structure (SR-XANES) spectroscopy, we successfully capture the 3D distribution of silver NPs (AgNPs) inside a single human monocyte (THP-1), associated with the chemical transformation of silver. The results reveal that the cytotoxicity of AgNPs is largely due to the chemical transformation of particulate silver from elemental silver (Ag(0))n, to Ag(+) ions and Ag-O-, then Ag-S- species. These results provide direct evidence in the long-lasting debate on whether the nanoscale or the ionic form dominates the cytotoxicity of silver nanoparticles. Further, the present approach provides an integrated strategy capable of exploring the chemical origins of cytotoxicity in metallic nanoparticles.

Visualising liver fibrosis by phase-contrast X-ray imaging in common bile duct ligated mice.

OBJECTIVES: To determine whether phase-contrast X-ray imaging can be used to visualise directly the accumulated extracellular matrix proteins associated with liver fibrosis in common bile duct ligated mice. METHODS: Twenty-six-week-old C57BL female mice were randomised into three groups. In groups 1 (n = 5) and 2 (n = 10), common bile duct ligation was conducted to produce secondary biliary cirrhosis. Mouse livers were then excised 15 (group 1) and 40 days (group 2) after the ligation of the common bile duct for imaging. In the control group, the livers of 5 mice were excised 40 days after the sham operation. Images were then acquired using the analyser crystal set at different positions of the rocking curve. RESULTS: The results show that the fibrotic septa and hepatic lobules enclosed by fibrotic septa can be visualised clearly at the whole organ level via phase-contrast X-ray imaging without any contrast agent. CONCLUSION: These results suggest that phase-contrast X-ray imaging can easily reveal the accumulated extracellular matrix proteins associated with liver fibrosis without using any contrast agent and has great potential in the study of liver fibrosis.

A 30 nm-resolution hard X-ray microscope with X-ray fluorescence mapping capability at BSRF.

A full-field transmission X-ray microscope (TXM) operating continuously from 5 keV to 12 keV with fluorescence mapping capability has been designed and constructed at the Beijing Synchrotron Radiation Facility, a first-generation synchrotron radiation facility operating at 2.5 GeV. Spatial resolution better than 30 nm has been demonstrated using a Siemens star pattern in both absorption mode and Zernike phase-contrast mode. A scanning-probe mode fluorescence mapping capability integrated with the TXM has been shown to provide 50 p.p.m. sensitivity for trace elements with a spatial resolution (limited by probing beam spot size) of 20 µm. The optics design, testing of spatial resolution and fluorescence sensitivity are presented here, including performance measurement results.