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Understanding microstructural and strain evolutions induced by noble gas production in the nuclear fuel matrix or plasma-facing materials is crucial for designing next generation nuclear reactors, as they are responsible for volumetric swelling and catastrophic failure. We describe a multimodal approach combining synchrotron-based nanoscale X-ray imaging techniques with atomic-scale electron microscopy techniques for mapping chemical composition, morphology and lattice distortion in a single crystal W induced by Kr irradiation. We report that Kr-irradiated single crystal W undergoes surface deformation, forming Kr containing cavities. Furthermore, positive strain fields are observed in Kr-irradiated regions, which lead to compression of underlying W matrix.

Quasi-two-dimensional (quasi-2D) materials hold promise for future electronics because of their unique band structures that result in electronic and mechanical properties sensitive to crystal strains in all three dimensions. Quantifying crystal strain is a prerequisite to correlating it with the performance of the device and calls for high resolution but spatially resolved rapid characterization methods. Here, we show that using fly-scan nano X-ray diffraction, we can accomplish a tensile strain sensitivity below 0.001% with a spatial resolution of better than 80 nm over a spatial extent of 100 μm on quasi-2D flakes of 1T-TaS2. Coherent diffraction patterns were collected from a ∼100 nm thick sheet of 1T-TaS2 by scanning a 12 keV focused X-ray beam across and rotating the sample. We demonstrate that the strain distribution around micron- and submicron-sized "bubbles" that are present in the sample may be reconstructed from these images. The experiments use state-of-the-art synchrotron instrumentation and will allow rapid and nonintrusive strain mapping of thin-film samples and electronic devices based on quasi-2D materials.

Journal of applied crystallography 53(4), 927 - 936 (2020). doi:10.1107/S1600576720006925, The ever-increasing brightness of synchrotron radiation sources demands improved X-ray optics to utilize their capability for imaging and probing biological cells, nano-devices and functional matter on the nanometre scale with chemical sensitivity. Hard X-rays are ideal for high-resolution imaging and spectroscopic applications owing to their short wavelength, high penetrating power and chemical sensitivity. The penetrating power that makes X-rays useful for imaging also makes focusing them technologically challenging. Recent developments in layer deposition techniques have enabled the fabrication of a series of highly focusing X-ray lenses, known as wedged multi-layer Laue lenses. Improvements to the lens design and fabrication technique demand an accurate, robust, in situ and at-wavelength characterization method. To this end, a modified form of the speckle tracking wavefront metrology method has been developed. The ptychographic X-ray speckle tracking method is capable of operating with highly divergent wavefields. A useful by-product of this method is that it also provides high-resolution and aberration-free projection images of extended specimens. Three separate experiments using this method are reported, where the ray path angles have been resolved to within 4 nrad with an imaging resolution of 45 nm (full period). This method does not require a high degree of coherence, making it suitable for laboratory-based X-ray sources. Likewise, it is robust to errors in the registered sample positions, making it suitable for X-ray free-electron laser facilities, where beam-pointing fluctuations can be problematic for wavefront metrology., Published by Wiley-Blackwell, [S.l.]

Over the last couple of decades, the synchrotron radiation research community has witnessed tremendous advancement in the field of X-ray imaging and microscopy. Continuing enhancement of the light ...

IEEE journal of photovoltaics 9(6), 1790-1799 (2019). doi:10.1109/JPHOTOV.2019.2942487, Strain within grains and at grain boundaries (GBs) in polycrystalline thin-film absorber layers limits the overall performance because of higher defect concentrations and band fluctuations. However, the nanoscale strain distribution in operational devices is not easily accessible using standard methods. X-ray nanodiffraction offers the unique possibility to evaluate the strain or lattice spacing at nanoscale resolution. Furthermore, the combination of nanodiffraction with additional techniques in the framework of multimodal scanning X-ray microscopy enables the direct correlation of the strain with material and device parameters such as the elemental distribution or local performance. This approach is applied for the investigation of the strain distribution in CdTe grains in fully operational photovoltaic solar cells. It is found that the lattice spacing in the (111) direction remains fairly constant in the grain cores but systematically decreases at the GBs. The lower strain at GBs is accompanied by an increase of the total tilt. These observations are both compatible with the inhomogeneous incorporation of smaller atoms into the lattice, and local stress induced by neighboring grains., Published by IEEE, New York, NY

Diffraction optics fabricated from multilayers offer an intriguing alternative to lithography-based zone plates due to their advantages of virtually limitless aspect ratio and extremely small feature size. However, other issues, intrinsic to thin-film deposition, such as film stress and deposition rate instability , for example, limit the total achievable aperture. Over the last decade, Multilayer Laue Lens (MLLs) have progressed from a mere curiosity with initial aperture sizes in the 3-10 m range, to real beamline-deployed optics with apertures in the 40-50 m range (X. Huang, et al., Scientific Reports 3, 3562 (2013); E. Nazaretski, et al., Rev. Sci. Instrum. 85, 033707 (2014); E. Nazaretski, et al., Journal of Synchrotron Radiation 24, 1113 (2017)). By optimizing deposition conditions and incorporating new materials, MLLs have now broken the 100 m thickness milestone. A flat WSi 2 /Al-Si MLL with a deposition thickness of 102 m, the largest MLL to date, is reviewed. New large aperture wedged MLLs (wMLL), which were first fabricated by APS in 2006 using the WSi 2 /Si material system, are presented which demonstrate high focusing efficiency across a broad energy range. These results confirm findings by other groups who have also independently fabricated wMLL (A. J. Morgan, et al., Scientific Reports 5, 9892 (2015); S. Bajt, et al., Nature Light: Science and Applications 7, 17162 (2017)) based on a similar material system.

Bicontinuous-nanostructured materials with a three-dimensionally (3D) interconnected morphology offer unique properties and potential applications in catalysis, biomedical sensing and energy storage. The new approach of solid-state interfacial dealloying (SSID) opens a route for fabricating bi-continuous metal–metal composites and porous metals at nano-/meso-scales via a self-organizing process driven by minimizing the system's free energy. Integrating SSID and thin film processing fully can open up a wide range of technological opportunities in designing novel functional materials; to-date, no experimental evidence has shown that 3D bi-continuous films can be formed with SSID, owing to the complexity of the kinetic mechanisms in thin film geometry and at nano-scales, despite the simple processing strategy in SSID. Here, we demonstrate that a fully-interconnected 3D bi-continuous structure can be achieved by this new approach, thin-film-SSID, using Fe–Ni film dealloyed by Mg film. The formation of a Fe–MgxNi bi-continuous 3D nano-structure was visualized and characterized via a multi-scale, multi-modal approach, combining electron transmission microscopy with synchrotron X-ray fluorescence nano-tomography and absorption spectroscopy. Phenomena involved with structural formation are discussed. These include surface dewetting, nano-size void formation among metallic ligaments, and interaction with a substrate. This work sheds light on the mechanisms of the SSID process, and sets a path for manufacturing of thin-film materials for future nano-structured metallic materials.

Using recent advances in X-ray microscopy, this study aimed to elucidate mechanisms of uptake, subcellular distribution, and translocation of functionalized CeO2 MNM (manufactured nanomaterials), having different charges, by tomato plants (Solanum lycopersicum cv Micro-Tom). We found that plant growth and Ce concentration in tissues were functions of surface charge and exposure concentration with root to shoot translocation being much greater for negatively charged CeO2 than positive or neutral CeO2. Mechanisms of entry into roots and translocation within plants were examined using X-ray nano- and microprobes. There were dramatic differences in the tissue and subcellular distributions of Ce in plant roots exposed to dextran-coated CeO2 nanoparticles conjugated with positive, neutral and negative functional groups. Positively charged CeO2 remained mainly bound to the epidermis of the root with little present in the apoplast or cytoplasm. Negatively charged CeO2 was found in the cytoplasm throughout the root cross section, and negatively charged CeO2 was found within the apoplast in the cortex and both the apoplast and the cytoplasm in the vasculature. Neutral CeO2 likely entered through the gaps between epidermal cells being sloughed off during root growth and penetrated deeper into the interior of the roots (vasculature) via a combination of apoplastic and symplastic transport. Evidence of symplastic Ce transport was observed with the neutrally and negatively charged particles. We observed evidence of endocytosis as the mechanism for entry into the symplast allowing for entry into the xylem. This study provides critical information on how particle surface chemistry influences the biodistribution and cellular localization of nanomaterials in plants and is to date the highest resolution X-ray imaging of nanomaterials in plant cells.

Bragg coherent diffractive imaging (BCDI) is a noninvasive microscopy technique that can visualize the morphology and internal lattice deviations of crystals with nanoscale spatial resolution and picometer deformation sensitivity. While BCDI has been successfully applied in various studies of materials, it is less successful for highly strained crystals. Specifically, it is difficult to correctly reconstruct the electron density of a highly strained object using conventional phase retrieval algorithms. Although various algorithms have been developed to overcome this challenge, most of them require a priori knowledge that is not always available in practice. Here we report a phase retrieval workflow that can invert diffraction patterns from multiple Bragg peaks simultaneously. The workflow is explored via simulated diffraction from crystals with various strain conditions. Reconstructions from the workflow consistently demonstrate more accurate electron density maps, in comparison with the conventional method. For highly strained crystals, the workflow improves the reliability and consistency of BCDI phase retrieval significantly.

We report on a developed micromachined silicon platform for the precise assembly of 2D multilayer Laue lenses (MLLs) for high-resolution X-ray microscopy. The platform is 10 &times, 10 mm2 and is fabricated on ~500 &micro, m thick silicon wafers through multiple steps of photolithography and deep reactive-ion etching. The platform accommodates two linear MLLs in a pre-defined configuration with precise angular and lateral position control. In this work, we discuss the design and microfabrication of the platform, and characterization regarding MLLs assembly, position control, repeatability, and stability. The results demonstrate that a micromachined platform can be used for the assembly of a variety of MLLs with different dimensions and optical parameters. The angular misalignment of 2D MLLs is well controlled in the range of the designed accuracy, down to a few millidegrees. The separation distance between MLLs is adjustable from hundreds to more than one thousand micrometers. The use of the developed platform greatly simplifies the alignment procedure of the MLL optics and reduces the complexity of the X-ray microscope. It is a significant step forward for the development of monolithic 2D MLL nanofocusing optics for high-resolution X-ray microscopy.

High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials’ thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient’s stabilization effect remains elusive because it is inseparable from nickel’s valence gradient effect. To isolate nickel’s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi0.8Mn0.1Co0.1O2 material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni3+ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials., High-nickel content cathode materials suffer issues of structural and surface instability. Herewith authors show that introduction of a nickel valence gradient enhances the thermal and cycle stability of high-nickel content cathode materials.

A hard X-ray scanning microscope installed at the Hard X-ray Nanoprobe beamline of the National Synchrotron Light Source II has been designed, constructed and commissioned. The microscope relies on a compact, high stiffness, low heat dissipation approach and utilizes two types of nanofocusing optics. It is capable of imaging with ∼15 nm × 15 nm spatial resolution using multilayer Laue lenses and 25 nm × 26 nm resolution using zone plates. Fluorescence, diffraction, absorption, differential phase contrast, ptychography and tomography are available as experimental techniques. The microscope is also equipped with a temperature regulation system which allows the temperature of a sample to be varied in the range between 90 K and 1000 K. The constructed instrument is open for general users and offers its capabilities to the material science, battery research and bioscience communities.

A multimodal in situ nanofocused X-ray microscopy approach is demonstrated and applied to a working polycrystalline thin film solar cell that revealed chemical, structural and electronic heterogeneity from a single measurement., The factors limiting the performance of alternative polycrystalline solar cells as compared with their single-crystal counterparts are not fully understood, but are thought to originate from structural and chemical heterogeneities at various length scales. Here, it is demonstrated that multimodal focused nanobeam X-ray microscopy can be used to reveal multiple aspects of the problem in a single measurement by mapping chemical makeup, lattice structure and charge collection efficiency simultaneously in a working solar cell. This approach was applied to micrometre-sized individual grains in a Cu(In,Ga)Se2 polycrystalline film packaged in a working device. It was found that, near grain boundaries, collection efficiency is increased, and that in these regions the lattice parameter of the material is expanded. These observations are discussed in terms of possible physical models and future experiments.

Incorporation of foreign elements into the cathode material is broadly adopted by both academia and industry to improve the battery performance. The lack of an in-depth understanding for the underlying mechanism, however, makes it a largely try-and-error process with unsatisfactory efficiency and effectiveness. This is particularly true for the electrochemical reaction kinetics that is heterogeneous over a broad range of length scales and is determined collectively by the cathode’s electronic structure, lattice configuration, and micro-morphology. Here we unveiled a facet-dependent dopant segregation effect in Zr-modified single-crystal LiNi0.6Co0.2Mn0.2O2 cathode. By forming kinetically favored corners on the cathode particles, the presence of a trace amount of Zr critically modulates the mesoscale reaction kinetics. Our findings suggest that a delicately controlled dopant distribution is a viable strategy for designing the next-generation battery cathode with superior structural and chemical robustness.

International audience; III-As nanowires are candidates for near infrared light emitters and detectors that can be directly integrated onto silicon. However, nanoscale to microscale variations in structure, composition, and strain within a given nanowire, as well as variations between nanowires, pose challenges to correlating microstructure with device performance. In this work, we utilize coherent nano-focused x-rays to characterize stacking defects and strain in a single InGaAs nanowire supported on Si. By reconstructing diffraction patterns from the 2110 Bragg peak, we show that the lattice orientation varies along the length of the wire, while the strain field along the cross-section is largely unaffected, leaving the band structure unperturbed. Diffraction patterns from the 0110 Bragg peak are reproducibly reconstructed to create three-dimensional images of stacking defects and associated lattice strains, revealing sharp planar boundaries between different crystal phases of wurtzite (WZ) structure that contribute to charge carrier scattering. Phase retrieval is made possible by developing multi-angle Bragg projection ptychography (maBPP) to accommodate coherent nanodiffraction patterns measured at arbitrary overlapping positions at multiple angles about a Bragg peak, eliminating the need for scan registration at different angles. The penetrating nature of x-ray radiation, together with the relaxed constraints of maBPP, will enable in operado imaging of nanowire devices.

X-Ray Microscopy 2018, Saskatoon, Canada, 19 Aug 2018 - 24 Aug 2018; Microscopy and microanalysis 24(S2), 434 - 435 (2018). doi:10.1017/S1431927618014423, Published by Cambridge University Press

We discuss misalignment-induced aberrations in a pair of crossed multilayer Laue lenses used for achieving a nanometer-scale x-ray point focus. We thoroughly investigate the impacts of two most important contributions, the orthogonality and the separation distance between two lenses. We find that misalignment in the orthogonality results in astigmatism at 45° and other inclination angles when coupled with a separation distance error. Theoretical explanation and experimental verification are provided. We show that to achieve a diffraction-limited point focus, accurate alignment of the azimuthal angle is required to ensure orthogonality between two lenses, and the required accuracy is scaled with the ratio of the focus size to the aperture size.

We report scanning hard x-ray imaging with a monolithic focusing optic consisting of two multilayer Laue lenses (MLLs) bonded together. With optics pre-characterization and accurate control of the bonding process, we show that a common focal plane for both MLLs can be realized at 9.317 keV. Using bonded MLLs, we obtained a scanning transmission image of a star test pattern with a resolution of 50 × 50 nm2. By applying a ptychography algorithm, we obtained a probe size of 17 × 38 nm2 and an object image with a resolution of 13 × 13 nm2. The significant reduction in alignment complexity for bonded MLLs will greatly extend the application range in both scanning and full-field x-ray microscopies.

The article presents a theoretical study on dynamic artefacts in the reconstruction of Bragg coherent diffractive imaging using an iterative phase retrieval algorithm., This article reports a theoretical study on the reconstruction artefacts in Bragg coherent diffractive imaging caused by dynamical diffraction effects. It is shown that, unlike the absorption and refraction effects that can be corrected after reconstruction, dynamical diffraction effects have profound impacts on both the amplitude and the phase of the reconstructed complex object, causing strong artefacts. At the dynamical diffraction limit, the reconstructed shape is no longer correct, as a result of the strong extinction effect. Simulations for hemispherical particles of different sizes show the type, magnitude and extent of the dynamical diffraction artefacts, as well as the conditions under which they are negligible.

This publisher's note corrects an error in Eq. (3) of Opt. Lett.44, 503 (2019).OPLEDP0146-959210.1364/OL.44.000503.

We developed a scanning hard x-ray microscope using a new class of x-ray nano-focusing optic called a multilayer Laue lens and imaged a chromosome with nanoscale spatial resolution. The combination of the hard x-ray’s superior penetration power, high sensitivity to elemental composition, high spatial-resolution and quantitative analysis creates a unique tool with capabilities that other microscopy techniques cannot provide. Using this microscope, we simultaneously obtained absorption-, phase- and fluorescence-contrast images of Pt-stained human chromosome samples. The high spatial-resolution of the microscope and its multi-modality imaging capabilities enabled us to observe the internal ultra-structures of a thick chromosome without sectioning it.

We report multimodal scanning hard x-ray imaging with spatial resolution approaching 10 nm and its application to contemporary studies in the field of material science. The high spatial resolution is achieved by focusing hard x-rays with two crossed multilayer Laue lenses and raster-scanning a sample with respect to the nanofocusing optics. Various techniques are used to characterize and verify the achieved focus size and imaging resolution. The multimodal imaging is realized by utilizing simultaneously absorption-, phase-, and fluorescence-contrast mechanisms. The combination of high spatial resolution and multimodal imaging enables a comprehensive study of a sample on a very fine length scale. In this work, the unique multimodal imaging capability was used to investigate a mixed ionic-electronic conducting ceramic-based membrane material employed in solid oxide fuel cells and membrane separations (compound of Ce0.8Gd0.2O2−x and CoFe2O4) which revealed the existence of an emergent material phase and quantified the chemical complexity at the nanoscale.

Multilayer Laue lenses (MLLs) are x-ray focusing optics with the potential to focus hard x-rays down to a single nanometer level. In order to achieve point focus, an MLL microscope needs to have the capability to perform tip-tilt motion of MLL optics and to hold the angular position for an extended period of time. In this work, we present a 2D tip-tilt system that can achieve an angular resolution of over 100 microdegree with a working range of 4°, by utilizing a combination of laser interferometer and mini retroreflector. The linear dimensions of the developed system are about 30 mm in all directions, and the thermal dissipation of the system during operation is negligible. Compact design and high angular resolution make the developed system suitable for MLL optics alignment in the next generation of MLL-based x-ray microscopes.

We report on the synthesis, stability, and local structure of In2O3 thin films grown via rf-magnetron sputtering and characterized by in-situ x-ray scattering and focused x-ray nanodiffraction. We find that In2O3 deposited onto (0 0 1)-oriented single crystal yttria-stabilized zirconia substrates adopts a Stranski–Krastanov growth mode at a temperature of 850 °C, resulting in epitaxial, truncated square pyramids with (1 1 1) side walls. We find that at this temperature, the pyramids evaporate unless they are stabilized by a low flux of In2O3 from the magnetron source. We also find that the internal lattice structure of one such pyramid is made up of differently strained volumes, revealing local structural heterogeneity that may impact the properties of In2O3 nanostructures and films.

In this study,we present a numerical framework for modeling three-dimensional (3D) diffraction data in Bragg coherent diffraction imaging (BraggCDI) experiments and evaluating the quality of obtained 3D complex-valued real-space images recovered by reconstruction algorithms under controlled conditions. The approach is used to systematically explore the performance and the detection limit of this phase-retrieval-based microscopy tool. The numerical investigation suggests that the superb performance of Bragg CDI is achieved with an oversampling ratio above 30 and a detection dynamic range above 6 orders. The observed performance degradation subject to the data binning processes is also studied. This numerical tool can be used to optimize experimental parameters and has the potential to significantly improve the throughput of Bragg CDI method.

We report our experiences with conducting ptychography simultaneously with the X-ray fluorescence measurement using the on-the-fly mode for efficient multi-modality imaging. We demonstrate that the periodic artifact inherent to the raster scan pattern can be mitigated using a sufficiently fine scan step size to provide an overlap ratio of >70%. This allows us to obtain transmitted phase contrast images with enhanced spatial resolution from ptychography while maintaining the fluorescence imaging with continuous-motion scans on pixelated grids. This capability will greatly improve the competence and throughput of scanning probe X-ray microscopy.

The focusing performance of a multilayer Laue lens (MLL) with 43.4 μm aperture, 4 nm finest zone width and 4.2 mm focal length at 12 keV was characterized with X-rays using ptychography method. The reconstructed probe shows a full-width-at-half-maximum (FWHM) peak size of 11.2 nm. The obtained X-ray wavefront shows excellent agreement with the dynamical calculations, exhibiting aberrations less than 0.3 wave period, which ensures the MLL capable of producing a diffraction-limited focus while offering a sufficient working distance. This achievement opens up opportunities of incorporating a variety of in-situ experiments into ultra high-resolution X-ray microscopy studies.

Replacing organic liquid electrolyte with inorganic solid electrolytes (SE) can potentially address the inherent safety problems in conventional rechargeable batteries. However, solid-state batteries (SSBs) have been plagued by the relatively low ionic conductivity of SEs and large charge-transfer resistance between electrode and SE. Here, a new design strategy is reported for improving the ionic conductivity of SE by self-forming a composite material. An optimized Na+ ion conducting composite electrolyte derived from the Na1+ n Zr2Si n P3− n O12 NASICON (Na Super Ionic Conductor) structure is successfully synthesized, yielding ultrahigh ionic conductivity of 3.4 mS cm−1 at 25 °C and 14 mS cm−1 at 80 °C. On the other hand, in order to enhance the charge-transfer rate at the electrode/electrolyte interface, an interface modification strategy is demonstrated by utilization of a small amount of nonflammable and nonvolatile ionic liquid (IL) at the cathode side in SSBs. The IL acts as a wetting agent, enabling a favorable interface kinetic in SSBs. The Na3V2(PO4)3/IL/SE/Na SSB exhibits excellent cycle performance and rate capability. A specific capacity of ≈90 mA h g−1 is maintained after 10 000 cycles without capacity decay under 10 C rate at room temperature. This provides a new perspective to design fast ion conductors and fabricate long life SSBs.

We have developed an experimental approach to bond two independent linear Multilayer Laue Lenses (MLLs) together. A monolithic MLL structure was characterized using ptychography at 12 keV photon energy, and we demonstrated 12 nm and 24 nm focusing in horizontal and vertical directions, respectively. Fabrication of 2D MLL optics allows installation of these focusing elements in more conventional microscopes suitable for x-ray imaging using zone plates, and opens easier access to 2D imaging with high spatial resolution in the hard x-ray regime.