Synchrotron X-ray Tomography Research Articles

Dendritic deformation modes in additive manufacturing revealed by operando x-ray diffraction

Dynamic solidification behavior during metal additive manufacturing directly influences the as-built microstructure, defects, and mechanical properties of printed parts. How the formation of these features is driven by temperature variation (e.g., thermal gradient magnitude and solidification front velocity) has been studied extensively in metal additive manufacturing, with synchrotron x-ray imaging becoming a critical tool to monitor these processes. Here, we extend these efforts to monitoring full thermomechanical deformation during solidification through the use of operando x-ray diffraction during laser melting. With operando diffraction, we analyze thermomechanical deformation modes such as torsion, bending, fragmentation, assimilation, oscillation, and interdendritic growth. Understanding such phenomena can aid the optimization of printing strategies to obtain specific microstructural features, including localized misorientations, dislocation substructure, and grain boundary character. The interpretation of operando diffraction results is supported by post-mortem electron backscatter diffraction analyses.

Deformation evolves from shear to extensile in rocks due to energy optimization

Determining how fracture network development leads to macroscopic failure in heterogeneous materials may help estimate the timing of failure in rocks in the upper crust as well as in engineered structures. The proportion of extensile and shear deformation produced by fracture development indicates the appropriate failure criteria to apply, and thus is a key constraint in such an effort. Here, we measure the volume proportion of extensile and shear fractures using the orientation of the fractures that develop in triaxial compression experiments in which fractures are identified using dynamic in situ synchrotron X-ray imaging. The fracture orientations transition from shear to extensile approaching macroscopic, system-size failure. Numerical models suggest that this transition occurs because the fracture networks evolve in order to optimize the total mechanical efficiency of the system. Our results provide a physical interpretation of the empirical internal friction coefficient in rocks.

Revealing the Multifaceted Impacts of Electrode Modifications for Vanadium Redox Flow Battery Electrodes.

Carbon electrodes are one of the key components of vanadium redox flow batteries (VRFBs), and their wetting behavior, electrochemical performance, and tendency to side reactions are crucial for cell efficiency. Herein, we demonstrate three different types of electrode modifications: poly(o-toluidine) (POT), Vulcan XC 72R, and an iron-doped carbon-nitrogen base material (Fe-N-C + carbon nanotube (CNT)). By combining synchrotron X-ray imaging with traditional characterization approaches, we give thorough insights into changes caused by each modification in terms of the electrochemical performance in both half-cell reactions, wettability and permeability, and tendency toward the hydrogen evolution side reaction. The limiting performance of POT and Vulcan XC 72R could mainly be ascribed to hindered electrolyte transport through the electrode. Fe-N-C + CNT displayed promising potential in the positive half-cell with improved electrochemical performance and wetting behavior but catalyzed the hydrogen evolution side reaction in the negative half-cell.

Boosting Potassium Storage via Multifunctional Interface with High Lattice-Matching.

Atomic-scale interface engineering is a prominent strategy to address the large volume expansions and sluggish redox kinetics for reinforcing K-storage. Here, to accelerate charge transport and lower the activation energy, dual carbon-modified interfacial regions are synthesized with high lattice-matching degree, which is formed from a CoSe2 /FeSe2 heterostructure coated onto hollow carbon fibers. State-of-the-art characterization techniques and theoretical analysis, including ex-situ soft X-ray absorption spectroscopy, synchrotron X-ray tomography, ultrasonic transmission mapping, and density functional theory, are conducted to probe local atomic structure evolution, mechanical degradation mechanisms, and ion/electron migration pathways. The results suggest that the heterostructure composed of the same crystal system and space group can sharply regulate the redox kinetics of transition metal selenium and dual carbon-modified approach can tailor physicochemical degradation. Overall, this work presents the design of a stable heterojunction synergistic superior hollow carbon substrate, inspiring a pathway of interface engineering strategy toward high-performance electrode.

Understanding the formation of “false friends” (hidden lack of fusion defects) in laser beam welding by means of high-speed synchrotron X-ray imaging

This paper provides a fundamental understanding of “false friend” formation, i.e., hidden defects associated with lack of fusion, using an experimental setup that allowed an insight into the processing zone based on high-speed synchrotron X-ray imaging. The setup enabled the welding of a lap joint of AISI 304 high-alloy steel sheets (X5CrNi18-10/1.4301), with the ability to adjust different gap heights between top and bottom sheet (up to 0.20 mm) and to acquire high-speed X-ray images at 100 kHz simultaneously with the welding process. On this basis, a time-resolved description of the “false friend” formation can be provided by visualizing the interaction between keyhole and melt pool during laser welding and solidification processes within the gap area. The bridgeability of the gap was limited due to the gap height and insufficient melt supply leading to the solidification of the bridge. The distance between the solidified bridge and the keyhole increased with time, while the keyhole and melt pool dynamics initiated the formation of new melt bridges whose stability was defined by melt flow conditions, surface tension, and gap heights. The alternating formation and solidification of melt bridges resulted in entrapped areas of lacking fusion within the weld, i.e., “false friends.” Finally, based on the results of this study, a model concept is presented that concludes the main mechanisms of “false friend” formation.

In situ synchrotron x-ray imaging and diffraction study of additively manufactured AlSi10Mg alloy under uniaxial tension

In situ synchrotron x-ray imaging and diffraction are used to investigate deformation dynamics in two kinds of additively manufactured AlSi10Mg with different pore configurations. The pre-existing pore configurations are characterized with synchrotron x-ray computed tomography. The specimens are subjected to tensile loading along the build direction and the longitudinal direction. Bulk stress–strain curves (macroscale), strain fields (mesoscale) and x-ray diffraction patterns (microscale) are obtained simultaneously. Scanning electron microscopy characterization is performed as a complement. For the small-pored AlSi10Mg, preferred orientations of pores lead to anisotropic ductility, and only ductile dimples are observed. For the large-pored AlSi10Mg, ductility loss is significant due to its higher porosity, and no remarkable anisotropy is found; both ductile and brittle fracture features are identified. For both types of AlSi10Mg, strain localization occurs around the pores. At the lattice scale, the Al matrix deforms plastically but the Si phase is still strained elastically, and thus, significant stress concentration occurs in the Si phase for the small-pored AlSi10Mg, while stress is more evenly partitioned between the Al matrix and the Si phase for the large-pored AlSi10Mg.

Towards an Understanding of the Challenges in Laser Beam Welding of Copper – Observation of the Laser-Matter Interaction Zone in Laser Beam Welding of Copper and Steel Using in Situ Synchrotron X-Ray Imaging

The increasing demand for contacting applications in electric components such as batteries, power electronics and electric drives is boosting the use of laser-based copper processing. Laser beam welding is a key for an efficient and high-quality electric vehicle production due to its local, non-contact energy input and high automation capability enabling reproducible weld quality. Nevertheless, a major challenge in process design is the combination of energy-efficiency and precise process guidance with regard to weld seam depth and defect prevention (i.e. spatter, melt ejections), partly caused by the high thermal conductivity of copper. High power lasers in the near infrared range and emerging visible laser beam sources with excellent beam quality can provide a suitable joining solution for this purpose. However, the underlying physical phenomena are currently only partly understood and a reflection on the challenges of laser beam welding of copper compared to well researched steel processing has not yet been carried out. In order to improve the understanding of the effect of the different material properties and the influence of process parameters on the vapor capillary and melt pool geometry in laser beam welding, in situ synchrotron investigations on Cu-ETP and S235 using 515 and 1030 nm laser sources were conducted. The material phase contrast analysis was successfully used to distinguish vapor capillary and melt pool phase boundaries during the welding process with high spatial and temporal resolution up to 5 kHz. A significantly different vapor capillary geometry and sensitivity to parameter variation were found between the steel and copper material. In addition, the visualization of characteristic melt flows revealed different melt pool dynamics and a pronounced eddy close to the melt pool surface for copper, which is assumed to be causal for the observation of pronounced spatter formation during copper welding in a certain process window.

Evaluation of high intensity synchrotron radiation x-ray imaging using Si crystals with lapped surface at 33.3 keV.

In x-ray imaging methods, such as synchrotron radiation microangiography, the x-ray intensity has become more important in recent years for real-time dynamic observations to evaluate temporal changes in samples. Many synchrotron radiation facilities use x-rays monochromated by diffraction from perfect Si crystals to improve the spatial resolution of x-ray images and obtain detailed information about a sample. In this paper, monochromatic synchrotron x-ray images were acquired using Si crystals lapped with abrasives to enhance the x-ray intensity using white synchrotron radiation x-rays for observing dynamic changes in samples. The x-ray intensity, spatial resolution, and contrast noise ratio (CNR) in the acquired x-ray images were quantitatively evaluated using a state-of-the-art high-spatial-resolution detector. The x-ray intensity was substantially increased by a factor of ∼8 when a lapped Si crystal was used. When the lapped Si crystal was used, the spatial resolution of x-ray images in the diffraction-plane direction was ∼70% lower than when an etched Si crystal was used at a spatial resolution of 10 lp/mm. By contrast, the CNR in x-ray images, which is important for observing the interior of a sample, increased threefold when a contrast agent containing iodine at a concentration of 38 wt. % was used. It was confirmed that the combination of white synchrotron radiation x-rays and a lapped crystal produces an intense monochromatic x-ray, providing an important evaluation for the use of optics for each research purpose.

Localized keyhole pore prediction during laser powder bed fusion via multimodal process monitoring and X-ray radiography

Systematic fault detection and control during laser powder bed fusion (L-PBF) has been a long-standing objective for system manufacturers and researchers in the additive manufacturing (AM) industry. This manuscript investigates a data fusion approach for detection of keyhole porosity formation during laser irradiation of Ti-6Al-4V substrates by concurrent recording of thermally induced optical emission measured using both off-axis and coaxial photodiode sensors, and acoustic emission. Subsurface defect formation was monitored via high-speed synchrotron X-ray imaging at 20,000 frames per second, enabling temporal registration of keyhole pore formation events to the monitoring signals at a resolution of 50 µs. We developed data fusion machine learning (ML) models for localized prediction of keyhole pore formation at various time scales ranging from 0.5 ms to 2 ms. The signal segments were featurized using two independent approaches: (1) power spectral density (PSD) and (2) highly comparative time series analysis (HCTSA) framework. The extracted features from different sensor modalities were fused together to construct a multimodal feature space and sequential feature selection was used to determine the most informative features for training the ML models. The predictive performance was evaluated for three classifying algorithms: Support Vector Machine (SVM), K-Nearest Neighbor (KNN), and Gaussian Naive Bayes (GNB). As a result, pore formation events were predicted with up to 0.95 F1-score, 1.0 recall and 0.94 accuracy. The most heavily weighted features indicate that model performance is chiefly governed by the acoustic monitoring signal, with a secondary contribution from the optical emission sensors.

Multimodal and multiscale characterization reveals how tendon structure and mechanical response are altered by reduced loading.

Tendons are collagen-based connective tissues where the composition, structure and mechanics respond and adapt to the local mechanical environment. Adaptation to prolonged inactivity can result in stiffer tendons that are more prone to injury. However, the complex relation between reduced loading, structure, and mechanical performance is still not fully understood. This study combines mechanical testing with high-resolution synchrotron X-ray imaging, scattering techniques and histology to elucidate how reduced loading affects the structural properties and mechanical response of rat Achilles tendons on multiple length scales. The results show that reduced in vivo loading leads to more crimped and less organized fibers and this structural inhomogeneity could be the reason for the altered mechanical response. Unloading also seems to change the fibril response, possibly by altering the strain partitioning between hierarchical levels, and to reduce cell density. This study elucidates the relation between in vivo loading, the Achilles tendon nano-, meso‑structure and mechanical response. The results provide fundamental insights into the mechanoregulatory mechanisms guiding the intricate biomechanics, tissue structural organization, and performance of complex collagen-based tissues. STATEMENT OF SIGNIFICANCE: Achilles tendon properties allow a dynamic interaction between muscles and tendon and influence force transmission during locomotion. Lack of physiological loading can have dramatic effects on tendon structure and mechanical properties. We have combined the use of cutting-edge high-resolution synchrotron techniques with mechanical testing to show how reduced loading affects the tendon on multiple hierarchical levels (from nanoscale up to whole organ) clarifying the relation between structural changes and mechanical performance. Our findings set the first step to address a significant healthcare challenge, such as the design of tailored rehabilitations that take into consideration structural changes after tendon immobilization.

Two-layer cathode architecture for high-energy density and high-power density solid state batteries

Solid state batteries with high-energy density and high-power density require the development of thick and energy dense cathodes. Structured cathode electrodes with a double-layer configuration were enabled using a freeze tape casting technique. A bottom dense layer was utilized to enhance the energy density whereas a top porous layer with vertically aligned walls was utilized to enhance the power density. The porous structure of the power layer was achieved by ice templating this layer on top of the densified energy layer of the cathode. This configuration was found to better utilize the active material of the cathodes and was optimized using numerical simulation and computer modeling. Cells with Li metal anode and LiNi0.6Mn0.2Co0.2O2 (NMC622) at approximately 5 and 20 mg/cm2 were cycled at 70 °C at different C-rates. Poly(ethylene oxide) (PEO) with lithium bis-trifluoromethanesulfonimide (LiTFSI) was used for the catholyte and the solid-state electrolyte. The structured cathodes exhibited more than double capacity values as well as better Coulombic efficiency compared to non-structured (single-layer) thick cathodes. Synchrotron X-ray tomography and scanning electron microscopy were used to characterize the microstructure of the cathodes.

In situ X-ray imaging of electrochemical dissolution behavior at low current density of as-built additively manufactured AlSi10Mg alloy

Despite extensive research on electrochemical machining (ECM) for improving the surface quality of additively manufactured (AMed) metals, common problems of stray corrosion and uneven dissolution remain. Here, in-situ synchrotron X-ray imaging was firstly used for observing the dissolution behavior of as-built AlSi10Mg alloy at low current density. The bubble evolution, surface roughness and dissolved depth was investigated. The results demonstrated that surfaces with higher roughness exhibited a greater dissolution rate and consumed a larger proportion of electrons compared to smooth surfaces. The study also identified three distinct stages of surface roughness change at low current density, providing valuable insights for the development of ECM techniques for AMed parts.

Gas bubble coalescence in laser directed energy deposition of irregular HDH titanium alloy powder feedstock

In this study, the synchrotron X-ray imaging technique was used to investigate the coalescence of gas bubbles during laser directed energy deposition (L-DED) of irregular hydride-dehydride (HDH) titanium alloy particles onto a titanium alloy substrate. The objective is to better understand the coalescing mechanism of gas bubbles during the L-DED process of unique feedstock materials. The coalescence frequency of gas bubbles is the percentage of bubbles merging and is dependent on collision frequency and coalescence efficiency. Forces in the melt pool flow such as Marangoni forces, buoyancy force, vaporization pressure, and acoustic waves, along with the number of generated bubbles, were the major factors for increasing the collision frequency between bubbles. In addition, the random forest model determined that the diameter of the smaller bubble during collision was the most significant factor impacting the efficiency of coalescence, which was equal to 48% when the smaller diameter was larger than a threshold of 76 μm and 3.5% and when the diameter was smaller than 76 μm. The results also showed that 6.5% of the formed bubbles in the melt pool led to coalescence. Overall, this work can help mitigate pores, verify simulation models, and promote irregular or recycled powder feedstock as effective replacement to atomized feedstock.

Assessing continuum plasticity postulates with grain stress and local strain measurements in triaxially compressed sand

Critical state and continuum plasticity theories have been used in research and engineering practice in soil and rock mechanics for decades. These theories rely on postulated relationships between material stresses and strains. Some classical postulates include coaxiality between stress and strain rates, stress-dilatancy relationships, and kinematic assumptions in shear bands. Although numerical and experimental data have quantified the strains and grain kinematics in such experiments, little data quantifying grain stresses are available. Here, we report the first-known grain stress and local strain measurements in triaxial compression tests on synthetic quartz sands using synchrotron X-ray tomography and 3D X-ray diffraction. We use these data to examine the micromechanics of shear banding, with a focus on coaxiality, stress-dilatancy, and kinematics within bands. Our results indicate the following: 1) elevated deviatoric stress, strain, and stress ratios in shear bands throughout experiments; 2) coaxial principal compressive stresses and strains throughout samples; 3) significant contraction along shear bands; 4) vanishing volumetric strain but nonvanishing stress fluctuations throughout samples at all stages of deformation. Our results provide some of the first-known in situ stress and strain measurements able to aid in critically evaluating postulates employed in continuum plasticity and strain localization theories for sands.

Multi-resolution Correlative Ultrastructural and Chemical Analysis of Carious Enamel by Scanning Microscopy and Tomographic Imaging.

Caries, a major global disease associated with dental enamel demineralization, remains insufficiently understood to devise effective prevention or minimally invasive treatment. Understanding the ultrastructural changes in enamel is hampered by a lack of nanoscale characterization of the chemical spatial distributions within the dental tissue. This leads to the requirement to develop techniques based on various characterization methods. The purpose of the present study is to demonstrate the strength of analytic methods using a correlative technique on a single sample of human dental enamel as a specific case study to test the accuracy of techniques to compare regions in enamel. The science of the different techniques is integrated to genuinely study the enamel. The hierarchical structures within carious tissue were mapped using the combination of focused ion beam scanning electron microscopy with synchrotron X-ray tomography. The chemical changes were studied using scanning X-ray fluorescence (XRF) and X-ray wide-angle and small-angle scattering using a beam size below 80 nm for ångström and nanometer length scales. The analysis of XRF intensity gradients revealed subtle variations of Ca intensity in carious samples in comparison with those of normal mature enamel. In addition, the pathways for enamel rod demineralization were studied using X-ray ptychography. The results show the chemical and structural modification in carious enamel with differing locations. These results reinforce the need for multi-modal approaches to nanoscale analysis in complex hierarchically structured materials to interpret the changes of materials. The approach establishes a meticulous correlative characterization platform for the analysis of biomineralized tissues at the nanoscale, which adds confidence in the interpretation of the results and time-saving imaging techniques. The protocol demonstrated here using the dental tissue sample can be applied to other samples for statistical study and the investigation of nanoscale structural changes. The information gathered from the combination of methods could not be obtained with traditional individual techniques.

Combined operando and ex-situ monitoring of the Zn/electrolyte interface in Zn-ion battery systems

Operando optical microscopy enables imaging at the interface between the Zn electrode and the electrolyte of 1 M ZnSO4(aq) in the symmetrical Zn/Zn cells assembled as the pouch cells with the mechanical load of 0.8 MPa. The imaging was executed during cycling of Zn plating and stripping at the different current densities of 0.5, 1.0, 2.0, and 4.0 mA cm−2, and the areal capacity of 2 mAh·cm−2. When the current densities are below 4.0 mA cm−2, no intense Zn dendrites are observed. However, at 4.0 mA cm−2, the severe Zn dendrites can penetrate through the separator and cause short-circuiting. From the electrochemical perspective, the voltage profile of such system drops to almost zero volt. Both operando optical and ex-situ synchrotron X-ray imaging further prove the appearance of the Zn dendrites. By Raman spectroscopy and X-ray diffraction, the cycled Zn electrode surface contains passivation species of Zn4(OH)6SO4, ZnO, and Zn(OH)2 that could limit the active surface area for the Zn plating/stripping, accelerating the localized current density and favoring the growth of Zn dendrites. With the SiO2 additive of 0.5% w/v in 1 M ZnSO4(aq), the severe Zn dendrites disappear, as well as the cycled Zn/electrolyte interface becomes close to the pristine state; low degree of the Zn electrode roughness and the Zn surface passivation is noticed. The appearance of the claimed Zn surface morphology was also confirmed by Scanning Electron Microscopy (SEM). In turn, too low or too high SiO2 content in the electrolyte does not generate desirable effects. A high level of Zn dendrites and short circuiting are still recognized. Hence, both the operando and ex-situ characterizations can mutually validate the phenomena at the Zn/electrolyte interface.

The effectiveness of Ni microalloying on the microstructure and mechanical properties of low temperature In-35 wt%Sn/Cu solder joint

The effects of 0.05 wt%Ni additions on In-35 wt%Sn (In–35Sn) alloy on the ex-situ interfacial reactions, in-situ microstructures formation during solidification, and mechanical properties during reflow soldering on Cu substrate were systematically studied. Reaction of In–35Sn with Cu resulted in the formation of two intermetallic Cu3(Sn,In) layers were found at the interface. When Ni is added, Ni is participated in the interfacial (Cu,Ni)3(Sn,In) layer formed at the In–35Sn-0.05Ni/Cu interface, causing the morphology of the IMC layer at the solder side to become more refined. Adding Ni resulted in the degree of undercooling In–35Sn decreasing close to zero. The in-situ real-time synchrotron x-ray imaging confirmed that the presence of Ni is responsible for the spontaneous β-In3Sn grain nucleation and formation of equiaxed grain in the solder joint. The grain refinement on the (Cu,Ni)3(Sn,In) IMC layer in In–35Sn-0.05Ni/Cu solder joint leads to minor increment in the shear strength. This study demonstrated the effectiveness of Ni microalloying in low temperature In–35Sn/Cu solder joint in modifying the β-In3Sn dendrite growth at the bulk solder and the microstructure refinement at the interface of the solder joints, which could potentially enhance the overall joint strength.

In situ X-ray tomography study on internal damage evolution of solid propellant for carrier rockets

Nitrate Ester Plasticized Polyether (NEPE) propellant has been widely used for carrier rockets. However, the propellant is usually subjected to complex loads, changing the microstructures, which eventually affects its structural integrity. To elucidate the damage mechanism of the propellant, an in situ tensile testing rig with a maximum strain rate of 0.1 s−1 was developed with high-resolution synchrotron X-ray tomography. The internal microstructure and the resultant damage evolution have been characterized quantitatively. The mechanical behaviour of sampled propellant was extracted from the dynamic mechanical analysis. In addition, numerical simulation in terms of the spatial geometry of filler particles was performed in the framework of the micromechanical approach. To visualize the debonding process, a cohesive-zone model was employed to trace the debonding at the filler/matrix interface and then the damage evolution was characterized according to the cohesive behaviour. The results can assist in correlating the cohesive behaviour due to local heterogeneity with the macroscopic mechanical response for the NEPE propellant.

Fluid-Structure Interaction Modeling of the Aortic Hemodynamics in Adult Zebrafish: A Pilot Study Based on Synchrotron X-Ray Tomography

The zebrafish is increasingly used as a small animal model for cardiovascular disease, including vascular disorders. Nevertheless, a comprehensive biomechanical understanding of the zebrafish cardiovascular circulation is still lacking and possibilities for phenotyping the zebrafish heart and vasculature at adult - no longer optically transparent - stages are limited. To improve these aspects, we developed imaging-based 3D models of the cardiovascular system of wild-type adult zebrafish. In vivo high-frequency echocardiography and ex vivo synchrotron x-ray tomography were combined to build fluid-structure interaction finite element models of the fluid dynamics and biomechanics inside the ventral aorta. We successfully generated a reference model of the circulation in adult zebrafish. The dorsal side of the most proximal branching region was found as the location of highest first principal wall stress and was also a location of low wall shear stress. Reynolds number and oscillatory shear were very low compared to mice and humans. The presented wild-type results provide a first extensive biomechanical reference for adult zebrafish. This framework can be used for advanced cardiovascular phenotyping of adult genetically engineered zebrafish models of cardiovascular disease, showing disruptions of the normal mechano-biology and homeostasis. By providing reference values for key biomechanical stimuli (including wall shear stress and first principal stress) in wild-type animals, and a pipeline for image-based animal-specific computational biomechanical models, this study contributes to a more comprehensive understanding of the role of altered biomechanics and hemodynamics in heritable cardiovascular pathologies.

Controlling solute channel formation using magnetic fields

Solute channel formation introduces compositional and microstructural variations in a range of processes, from metallic alloy solidification, to salt fingers in ocean and water reservoir flows. Applying an external magnetic field interacts with thermoelectric currents at solid/liquid interfaces generating additional flow fields. This thermoelectric (TE) magnetohydrodynamic (TEMHD) effect can impact on solute channel formation, via a mechanism recently drawing increasing attention. To investigate this phenomenon, we combined in situ synchrotron X-ray imaging and Parallel-Cellular-Automata-Lattice-Boltzmann based numerical simulations to study the characteristics of flow and solute transport under TEMHD. Observations suggest the macroscopic TEMHD flow appearing ahead of the solidification front, coupled with the microscopic TEMHD flow arising within the mushy zone are the primary mechanisms controlling plume migration and channel bias. Two TE regimes were revealed, each with distinctive mechanisms that dominate the flow. Further, we show that grain orientation modifies solute flow through anisotropic permeability. These insights led to a proposed strategy for producing solute channel-free solidification using a time-modulated magnetic field.