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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 145 records · Page 8

Operando real-space imaging of a structural phase transformation in the high-voltage electrode LixNi0.5Mn1.5O4

Abstract Discontinuous solid-solid phase transformations play a pivotal role in determining the properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in Li x Ni 0.5 Mn 1.5 O 4 within an operational Li metal coin cell. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to a planar semi-coherent interface driven by dislocation dynamics. Our data indicates negligible kinetic limitations from interface propagation impacting the transformation kinetics, even at a discharge rate of C/2 (80 mA/g). This study highlights BCDI’s capability to decode complex operando diffraction data, offering exciting opportunities to study nanoscale phase transformations with various stimuli.

Sun, Yifei (ORCID:0000000295625120)↗

Enhancing scattering images for orientation recovery with diffusion map

We explore the possibility for orientation recovery in single-molecule coherent diffractive imaging with diffusion map. This algorithm approximates the Laplace-Beltrami operator, which we diagonalize with a metric that corresponds to the mapping of Euler angles onto scattering images. While suitable for images of objects with specific properties we show why this approach fails for realistic molecules. Here, we introduce a modification of the form factor in the scattering images which facilitates the orientation recovery and should be suitable for all recovery algorithms based on the distance of individual images. (C) 2016 Optical Society of America

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Three-dimensional imaging of dislocation dynamics during the hydriding phase transformation

Crystallographic imperfections can significantly alter material properties and responses to external stimuli, including solute induced phase transformations and crystal growth and dissolution . Despite recent progress in imaging defects using both electron and x-ray techniques, in situ three-dimensional imaging studies of defect dynamics, necessary to understand and engineer nanoscale processes, remains challenging. Here, we report in situ three-dimensional imaging of defect dynamics during the hydriding phase transformation of individual palladium nanocrystals by Bragg Coherent Diffractive Imaging (BCDI) . During constant pressure experiments, we observed that the phase transformation begins after the nucleation of dislocations in large (300 nm) particles. The 3D dislocation network shows that dislocations are close to the phase boundary. The 3D phase morphology resolved by BCDI suggests that the hydrogen-rich phase is more similar to a spherical cap on the hydrogen-poor phase than the core-shell model commonly assumed. We substantiate this conclusion using 3D phase field modeling and demonstrate how phase morphology affects the critical size for dislocation nucleation. We determine the size dependence of the transformation pressure for large (150-300 nm) palladium nanocrystals using variable pressure experiments. Our results reveal a pathway for solute induced structural phase transformations in nanocrystals and demonstrate BCDI as a novel method for understanding dislocation dynamics in phase transforming systems at the nanoscale.

36 MATERIALS SCIENCE↗

Coherent soft X-ray diffraction imaging of coliphage PR772 at the Linac coherent light source

Single-particle diffraction from X-ray Free Electron Lasers offers the potential for molecular structure determination without the need for crystallization. In an effort to further develop the technique, we present a dataset of coherent soft X-ray diffraction images of Coliphage PR772 virus, collected at the Atomic Molecular Optics (AMO) beamline with pnCCD detectors in the LAMP instrument at the Linac Coherent Light Source. The diameter of PR772 ranges from 65–70 nm, which is considerably smaller than the previously reported ~600 nm diameter Mimivirus. This reflects continued progress in XFEL-based single-particle imaging towards the single molecular imaging regime. As a result, the data set contains significantly more single particle hits than collected in previous experiments, enabling the development of improved statistical analysis, reconstruction algorithms, and quantitative metrics to determine resolution and self-consistency.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Atomic resolution coherent x-ray imaging with physics-based phase retrieval

Coherent x-ray imaging and scattering from accelerator based sources such as synchrotrons continue to impact biology, medicine, technology, and materials science. Many synchrotrons around the world are currently undergoing major upgrades to increase their available coherent x-ray flux by approximately two orders of magnitude. The improvement of synchrotrons may enable imaging of materials in operando at the atomic scale which may revolutionize battery and catalysis technologies. Current algorithms used for phase retrieval in coherent x-ray imaging are based on the projection onto sets method. These traditional iterative phase retrieval methods will become more computationally expensive as they push towards atomic resolution and may struggle to converge. Additionally, these methods do not incorporate physical information that may additionally constrain the solution. In this work, we present an algorithm which incorporates molecular dynamics into Bragg coherent diffraction imaging (BCDI). This algorithm, which we call PRAMMol (Phase Retrieval with Atomic Modeling and Molecular Dynamics) combines statistical techniques with molecular dynamics to solve the phase retrieval problem. We present several examples where our algorithm is applied to simulated coherent diffraction from 3D crystals and show convergence to the correct solution at the atomic scale.

47 OTHER INSTRUMENTATION↗

Utilizing broadband X-rays in a Bragg coherent X-ray diffraction imaging experiment

A method is presented to simplify Bragg coherent X-ray diffraction imaging studies of complex heterogeneous crystalline materials with a two-stage screening/imaging process that utilizes polychromatic and monochromatic coherent X-rays and is compatible with in situ sample environments. Coherent white-beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three-dimensional reciprocal-space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifying in situ chamber design. This approach was demonstrated with Au nanoparticles and will enable, for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.

36 MATERIALS SCIENCE↗

Ptychography at the Linac Coherent Light Source in a parasitic geometry

X-ray free-electron lasers (FELs) are being recognized as a powerful tool in an ever-increasing number of research fields, but are very limited as to the number of experiments that they can support. This work shows that more beamtime could be made available by using `parasitic' geometries, where a secondary experiment uses the X-ray beam that the primary experiment does not utilize. The first successful ptychography experiment, a scanning coherent diffractive imaging technique, in a parasitic geometry at an X-ray FEL is demonstrated. Utilizing the CXI hutch at the Linac Coherent Light Source (LCLS), it is shown that the obtained data are of high quality and that characterizing the beam using ptychography can be much faster than traditional imprinting methods.

42 ENGINEERING↗

Three-dimensional X-ray diffraction imaging of dislocations in polycrystalline metals under tensile loading

Abstract The nucleation and propagation of dislocations is an ubiquitous process that accompanies the plastic deformation of materials. Consequently, following the first visualization of dislocations over 50 years ago with the advent of the first transmission electron microscopes, significant effort has been invested in tailoring material response through defect engineering and control. To accomplish this more effectively, the ability to identify and characterize defect structure and strain following external stimulus is vital. Here, using X-ray Bragg coherent diffraction imaging, we describe the first direct 3D X-ray imaging of the strain field surrounding a line defect within a grain of free-standing nanocrystalline material following tensile loading. By integrating the observed 3D structure into an atomistic model, we show that the measured strain field corresponds to a screw dislocation.

36 MATERIALS SCIENCE↗

Focal Spot and Wavefront Sensing of an X-Ray Free Electron laser using Ronchi shearing interferometry

The Linac Coherent Light Source (LCLS) is an X-ray source of unmatched brilliance, that is advancing many scientific fields at a rapid pace. The highest peak intensities that are routinely produced at LCLS take place at the Coherent X-ray Imaging (CXI) instrument, which can produce spotsize at the order of 100 nm, and such spotsizes and intensities are crucial for experiments ranging from coherent diffractive imaging, non-linear x-ray optics and high field physics, and single molecule imaging. Nevertheless, a full characterisation of this beam has up to now not been performed. In this paper we for the first time characterise this nanofocused beam in both phase and intensity using a Ronchi Shearing Interferometric technique. The method is fast, in-situ, uses a straightforward optimization algoritm, and is insensitive to spatial jitter.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Influence of finite spatial coherence on ptychographic reconstruction

X-ray ptychography is an ultrahigh-resolution scanning coherent diffractive imaging technique, allowing quantitative measurements of extended samples and a simultaneous reconstruction of the illuminating wavefront. Recent development of the mixed-state reconstruction algorithm has triggered a certain interest in utilizing partially coherent X-ray sources for ptychography. Here, we study how finite spatial coherence influences the reconstructed image of a test structure. Our work shows that use of a highly coherent illumination provides images with better spatial resolution and fewer artefacts than the approach with partial coherence.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Time-resolved x-ray imaging of a laser-induced nanoplasma and its neutral residuals

The evolution of individual, large gas-phase xenon clusters, turned into a nanoplasma by a high power infrared laser pulse, is tracked from femtoseconds up to nanoseconds after laser excitation via coherent diffractive imaging, using ultra-short soft x-ray free electron laser pulses. A decline of scattering signal at high detection angles with increasing time delay indicates a softening of the cluster surface. Here we demonstrate, for the first time a representative speckle pattern of a new stage of cluster expansion for xenon clusters after a nanosecond irradiation. The analysis of the measured average speckle size and the envelope of the intensity distribution reveals a mean cluster size and length scale of internal density fluctuations. Furthermore, the measured diffraction patterns were reproduced by scattering simulations which assumed that the cluster expands with pronounced internal density fluctuations hundreds of picoseconds after excitation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Fluorescence intensity correlation imaging with high spatial resolution and elemental contrast using intense x-ray pulses

We theoretically investigate the fluorescence intensity correlation (FIC) of Ar clusters and Mo-doped iron oxide nanoparticles subjected to intense, femtosecond, and sub-femtosecond x-ray free-electron laser pulses for high-resolution and elemental contrast imaging. We present the FIC of Kα and Kαh emission in Ar clusters and discuss the impact of sample damage on retrieving high-resolution structural information and compare the obtained structural information with those from the coherent diffractive imaging (CDI) approach. We found that, while sub-femtosecond pulses will substantially benefit the CDI approach, few-femtosecond pulses may be sufficient for achieving high-resolution information with the FIC. Furthermore, we show that the fluorescence intensity correlation computed from the fluorescence of the Mo atoms in Mo-doped iron oxide nanoparticles can be used to image dopant distributions in the nonresonant regime.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Imaging Light‐Induced Migration of Dislocations in Halide Perovskites with 3D Nanoscale Strain Mapping

Abstract In recent years, halide perovskite materials have been used to make high‐performance solar cells and light‐emitting devices. However, material defects still limit device performance and stability. Here, synchrotron‐based Bragg coherent diffraction imaging is used to visualize nanoscale strain fields, such as those local to defects, in halide perovskite microcrystals. Significant strain heterogeneity within MAPbBr 3 (MA = CH 3 NH 3 + ) crystals is found in spite of their high optoelectronic quality, and both 〈100〉 and 〈110〉 edge dislocations are identified through analysis of their local strain fields. By imaging these defects and strain fields in situ under continuous illumination, dramatic light‐induced dislocation migration across hundreds of nanometers is uncovered. Further, by selectively studying crystals that are damaged by the X‐ray beam, large dislocation densities and increased nanoscale strains are correlated with material degradation and substantially altered optoelectronic properties assessed using photoluminescence microscopy measurements. These results demonstrate the dynamic nature of extended defects and strain in halide perovskites, which will have important consequences for device performance and operational stability.

36 MATERIALS SCIENCE↗

High Energy Micron Scale Pixel Hybrid Detector

The objective of this technology development project has been to fabricate and characterize a new X-ray area image sensor innovation designed for high efficiency detection and imaging of hard X-rays (>20 KeV) with micron scale pixel resolution. A key technology component consists of a monolithic hybrid X-ray detector built by layering an amorphous Selenium X-ray photoconductor film directly deposited on a small pitch (7.8μm) CMOS active pixel readout array. A specific goal of this work is to provide a new detector tool to researchers working with synchrotron light sources, to extend the depth of exploration into nanoscale structures, and do so cost effectively. Early generation X-ray imaging detector tools fail to provide adequate resolving power and efficiency at high energies and our innovation provides a solution. A majority of proposed phase I tasks were completed. Those tasks included, in collaboration with KA Imaging, successful fabrication of specified a-Se layers on a 1Mpixel CMOS readout array to create the direct hybrid X-ray imaging array, packaging of the imaging array, assembly of electronics into a shielded detector box, loading user interface software for camera control and image capture, and performing initial (no X-ray) detector evaluation at Farrier Microengineering facilities. After initial tests, extensive testing using the X-ray beam line 1-BM source at Argonne National Laboratory Advanced Photon Source(ANL-APS) was performed. Imaging performance studies were conducted at multiple X-ray beam energies. Studies included X-ray response vs. X-ray energy, vs. applied detector field strength (HV), response linearity vs. integration time, MTF vs. beam energy, image lag measurements, and micron scale resolution pattern target imaging. This high energy micron scale X-ray detection technology is a first of a kind to be evaluated at the ANL-APS and is supported by Dr. Antonino Miceli, head of the detector physics group. Accomplishments include the first successful demonstration of a 1Mpix amorphous Selenium on CMOS readout direct hybrid X-ray imaging detector at a DOE sponsored National Laboratory. Modeled performance predictions were confirmed, proving micron scale resolution as well as an order of magnitude increase in conversion efficiency over conventional scintillator detector performance. A discovery of evidence of propagation-based phase contrast edge enhancement was unplanned and will be exploited in future experiments. This phase 1 technology demonstration verifies the efficacy of proposed high energy micron scale pixel X-ray hybrid a-Se imaging array products. The new detector products will cost effectively replace early generation detector technologies that currently fail to address increasing demand for tools to study nano structures and physical processes at high X-ray energies above 20keV. For example, current systems for transmission X-ray microscopy have low efficiency and available large pixel (~55µm) direct detectors do not offer sufficient resolution for Bragg fringe imaging at high energies. This detector innovation will solve these inadequacies. The new detector technology will compete in a $50M scientific X-ray detector market, growing at 6%, and will benefit Microtomography(µCT), X-ray diffractometry (XRD), Coherent Diffraction Imaging (CDI) applications. One application specified by Dr. Miceli at ANL is the 3D reconstruction of compact crystals at high energies requires small pixel high efficiency X-ray detectors. Farrier Microengineering, working with colleagues at KA Imaging and the University of Waterloo, successfully achieved the critical objectives of the Phase I proposal. We have proven the technical feasibility of this innovation by building and successfully testing a 1Mpixel a-Se/CMOS hybrid direct X-ray imaging array. Our commercialization roadmap of detector products will be implemented during a phase II project. We will demonstrate a migration of the technology to larger detector array sizes, improved temporal performance with detector layer engineering, and improved environmental and operational stability. Manufacturability and cost effectiveness are key objectives and product designs will leverage current state of the art CMOS wafer fabrication quality and volume manufacturing economics.

36 MATERIALS SCIENCE↗

Operando Nanoscale Imaging of Electrochemically Induced Strain in a Locally Polarized Pt Grain

Developing new methods that reveal the structure of electrode materials under polarization is key to constructing robust structure-property relationships. However, many existing methods lack the spatial resolution in structural changes and fidelity to electrochemical operating conditions that are needed to probe catalytically relevant structures. Here, we combine a nanopipette electrochemical cell with three-dimensional X-ray Bragg coherent diffractive imaging to study how strain in a single Pt grain evolves in response to applied potential. During polarization, marked changes in surface strain arise from the Coulombic attraction between the surface charge on the electrode and the electrolyte ions in the electrochemical double layers, while the strain in the bulk of the crystal remains unchanged. The concurrent surface redox reactions have a strong influence on the magnitude and nature of the strain changes under polarization. In conclusion, our studies provide a powerful blueprint to understand how structural evolution influences electrochemical performance at the nanoscale.

36 MATERIALS SCIENCE↗

Operando Interaction and Transformation of Metastable Defects in Layered Oxides for Na‐Ion Batteries

Non-equilibrium defects often dictate the macroscopic properties of materials. They largely define the reversibility and kinetics of processes in intercalation hosts in rechargeable batteries. Recently, imaging methods have demonstrated that transient dislocations briefly appear in intercalation hosts during ion diffusion. Despite new discoveries, the understanding of impact, formation and self-healing mechanisms of transient defects, including and beyond dislocations, is lacking. Here, operando X-ray Bragg Coherent Diffractive Imaging (BCDI) and diffraction peak analysis capture the stages of formation of a unique metastable domain boundary, defect self-healing, and resolve the local impact of defects on ionic diffusion in Na x Ni 1-y MnyO 2 intercalation hosts in a charging sodium-ion battery. Results, applicable to a wide range of layered intercalation materials due to the shared nature of framework layers, elucidate new dynamics of transient defects and their connection to macroscopic properties, and suggest how to control the nanostructure dynamics.

36 MATERIALS SCIENCE↗