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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 55 records · Page 3

In-Situ Characterization Tools for Evaluating Radiation Tolerance and Elemental Migration in Perovskites

This paper discusses the in-situ characterization tools designed to assess radiation tolerance and elemental migration in perovskite materials. With the increasing use of perovskites in various technological applications, understanding their response to radiation exposure is paramount. Ion Beam Induced Charge (IBIC) emerges as a powerful tool for investigating the radiation tolerance of perovskites at the microscale. By employing focused ion beams, IBIC allows for the spatial mapping of charge carriers, offering insights into the material's electronic response to radiation-induced defects. This technique enables researchers to pinpoint areas of enhanced or suppressed charge collection, providing valuable information on the perovskite's intrinsic properties under irradiation. Rutherford Backscattering Spectrometry (RBS) complements the study by offering a quantitative analysis of elemental migration in perovskite materials. Through the precise measurement of backscattered ions, RBS provides a detailed understanding of the elemental composition and distribution within the perovskite lattice after radiation exposure. The integration of IBIC and RBS techniques in in-situ experiments enhances the comprehensive characterization of radiation effects on perovskites.

ion beams↗

Disentangling multiple scattering with deep learning: application to strain mapping from electron diffraction patterns

Abstract A fast, robust pipeline for strain mapping of crystalline materials is important for many technological applications. Scanning electron nanodiffraction allows us to calculate strain maps with high accuracy and spatial resolutions, but this technique is limited when the electron beam undergoes multiple scattering. Deep-learning methods have the potential to invert these complex signals, but require a large number of training examples. We implement a Fourier space, complex-valued deep-neural network, FCU-Net, to invert highly nonlinear electron diffraction patterns into the corresponding quantitative structure factor images. FCU-Net was trained using over 200,000 unique simulated dynamical diffraction patterns from different combinations of crystal structures, orientations, thicknesses, and microscope parameters, which are augmented with experimental artifacts. We evaluated FCU-Net against simulated and experimental datasets, where it substantially outperforms conventional analysis methods. Our code, models, and training library are open-source and may be adapted to different diffraction measurement problems.

36 MATERIALS SCIENCE↗

Multi-angle Precession Electron Diffraction (MAPED): A Versatile Approach to 4D-STEM Precession

Precession of a converged beam during acquisition of a 4D-STEM dataset improves strain, orientation, and phase mapping accuracy by averaging over continuous angles of illumination. Precession experiments usually rely on integrated systems, where automatic alignments lead to fast, high-quality results. The dependence of these experiments on specific hardware and software is evident even when switching to nonintegrated detectors on a precession tool, as experimental set-up becomes challenging and time-consuming. Here, we introduce multi-angle precession electron diffraction (MAPED): a method to perform electron diffraction by collecting sequential 4D-STEM scans at different incident beam tilts. The multiple diffraction datasets are averaged together postacquisition, resulting in a single dataset that minimizes the impact of the curvature and orientation of the Ewald sphere relative to the crystal under study. Our results demonstrate that even four additional tilts improved measurement of material properties, namely strain and orientation, as compared to single-tilt 4D-STEM experiments. We show the versatility and flexibility of our MAPED approach with data collected on a number of microscopes with different hardware configurations and a variety of detectors.

4D-STEM↗

Dimensionality-Mediated Semimetal-Semiconductor Transition in Ultrathin PtTe 2 Films

Platinum ditelluride (PtTe2), a type-II Dirac semimetal, remains semimetallic in ultrathin films down to just two tri-atomic layers (TLs) with a negative gap of -0.36 eV. Further reduction of the film thickness to a single TL induces a Lifshitz electronic transition to a semiconductor with a large positive gap of +0.79 eV. This transition is evidenced by experimental band structure mapping of films prepared by layer-resolved molecular beam epitaxy, and by comparing the data to first-principles calculations using a hybrid functional. The results demonstrate a novel electronic transition at the two-dimensional limit through film thickness control.

36 MATERIALS SCIENCE↗

An adaptive approach to machine learning for compact particle accelerators

Abstract Machine learning (ML) tools are able to learn relationships between the inputs and outputs of large complex systems directly from data. However, for time-varying systems, the predictive capabilities of ML tools degrade if the systems are no longer accurately represented by the data with which the ML models were trained. For complex systems, re-training is only possible if the changes are slow relative to the rate at which large numbers of new input-output training data can be non-invasively recorded. In this work, we present an approach to deep learning for time-varying systems that does not require re-training, but uses instead an adaptive feedback in the architecture of deep convolutional neural networks (CNN). The feedback is based only on available system output measurements and is applied in the encoded low-dimensional dense layers of the encoder-decoder CNNs. First, we develop an inverse model of a complex accelerator system to map output beam measurements to input beam distributions, while both the accelerator components and the unknown input beam distribution vary rapidly with time. We then demonstrate our method on experimental measurements of the input and output beam distributions of the HiRES ultra-fast electron diffraction (UED) beam line at Lawrence Berkeley National Laboratory, and showcase its ability for automatic tracking of the time varying photocathode quantum efficiency map. Our method can be successfully used to aid both physics and ML-based surrogate online models to provide non-invasive beam diagnostics.

97 MATHEMATICS AND COMPUTING↗

Focused Electron Beam-Based 3D Nanoprinting for Scanning Probe Microscopy: A Review

Scanning probe microscopy (SPM) has become an essential surface characterization technique in research and development. By concept, SPM performance crucially depends on the quality of the nano-probe element, in particular, the apex radius. Now, with the development of advanced SPM modes beyond morphology mapping, new challenges have emerged regarding the design, morphology, function, and reliability of nano-probes. To tackle these challenges, versatile fabrication methods for precise nano-fabrication are needed. Aside from well-established technologies for SPM nano-probe fabrication, focused electron beam-induced deposition (FEBID) has become increasingly relevant in recent years, with the demonstration of controlled 3D nanoscale deposition and tailored deposit chemistry. Moreover, FEBID is compatible with practically any given surface morphology. In this review article, we introduce the technology, with a focus on the most relevant demands (shapes, feature size, materials and functionalities, substrate demands, and scalability), discuss the opportunities and challenges, and rationalize how those can be useful for advanced SPM applications. As will be shown, FEBID is an ideal tool for fabrication/modification and rapid prototyping of SPM-tipswith the potential to scale up industrially relevant manufacturing.

36 MATERIALS SCIENCE↗

Mapping 1D Confined Electromagnetic Edge States in 2D Monolayer Semiconducting MoS 2 Using 4D-STEM

Here, four-dimensional (4D) scanning transmission electron microscopy is used to study the electric fields at the edges of 2D semiconducting monolayer MoS2. Sub-nanometer 1D features in the 2D electric field maps are observed at the outermost region along zigzag edges and also along nanowire MoS-terminated MoS 2 edges. Atomic-scale oscillations are detected in the magnitude of the 1D electromagnetic edge state, with spatial variations that depend on the specific periodic edge reconstructions. Electric field reconstructions, along with integrated differential phase contrast reconstructions, reveal the presence of low Z number atoms terminating many of the uniform edges, which are difficult to detect by annular dark field scanning transmission electron microscopy due to its limited dynamic range. Density functional theory calculations support the formation of periodic 1D edge states and also show that enhancement of the electric field magnitude can occur for some edge terminations. The experimentally observed electric fields at the edges are attributed to the absence of an opposing electric field from a nearest neighbor atom when the electron beam propagates through the 2D monolayer and interacts. These results show the potential of 4D-STEM to map the atomic scale structure and fluctuations of electric fields around edge atoms with different bonding states than bulk atoms in 2D materials, beyond conventional imaging.

2D materials↗

Method and system for in situ cross-linking of materials to produce three-dimensional features via electron beams from mobile accelerators

A method and system for in situ cross-linking of polymers, Bitumen, and other materials to produce arbitrary functional or ornamental three-dimensional features using electron beams provided by mobile accelerators comprises defining a desired pattern for imparting on a target area, mapping the target area, defining at least one discrete voxel in the target area according to the desired pattern to be imparted on the target area, assigning an irradiation value to each of the at least one discrete voxels, and delivering a dose of irradiation to each of the at least one discrete voxels according to the assigned irradiation value.

43 PARTICLE ACCELERATORS↗

Method and system for in situ cross-linking of materials to produce three-dimensional features via electron beams from mobile accelerators

A method and system for in situ cross-linking of polymers, Bitumen, and other materials to produce arbitrary functional or ornamental three-dimensional features using electron beams provided by mobile accelerators comprises defining a desired pattern for imparting on a target area, mapping the target area, defining at least one discrete voxel in the target area according to the desired pattern to be imparted on the target area, assigning an irradiation value to each of the at least one discrete voxels, and delivering a dose of irradiation to each of the at least one discrete voxels according to the assigned irradiation value.

Sauers, Aaron↗

Infrastructure-scale additive manufacturing using mobile electron accelerators

A method and system for in situ cross-linking of polymers, Bitumen, and other materials to produce arbitrary functional or ornamental three-dimensional features using electron beams provided by mobile accelerators comprises defining a desired pattern for imparting on a target area, mapping the target area, defining at least one discrete voxel in the target area according to the desired pattern to be imparted on the target area, assigning an irradiation value to each of the at least one discrete voxels, and delivering a dose of irradiation to each of the at least one discrete voxels according to the assigned irradiation value.

Sauers, Aaron↗

Beam controlled nano-robotic device

A system and method (referred to as a method) to fabricate nanorobots. The method generates a pixel map of an atomic object and identifies portions of the atomic object that form a nanorobot. The method stores those identifications in a memory. The method adjusts an electron beam to a noninvasive operating level and images the portions of the atomic object that form the nanorobot. The method executes a plurality of scanning profiles by the electron beam to form the nanorobot and detects nanorobot characteristics and their surroundings via the electron beam in response to executing the plurality of scanning profiles.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Magnetic Field Mapping Design for the MOLLER Spectrometer Magnets at Jefferson Lab

The Thomas Jefferson National Accelerator Facility (JLab) has developed a unique spectrometer system to study the weak interaction between electrons. The "Measurement of Lepton-Lepton Electroweak Reaction" (MOLLER) experiment, utilizing JLab's recent 12 GeV electron beam upgrade, is scheduled to operate for three years. Central to the MOLLER experiment are five water-cooled toroidal magnets, each with a unique geometry and seven-fold symmetry, designed to focus the particles. These magnets generate the magnetic field needed to separate incident beam electrons scattered from target electrons (Møller scattering) and protons (elastic e-p scattering) within a liquid hydrogen target. Here, this paper details the magnet field measuring technique developed to map all five MOLLER toroidal magnets at multiple locations inside and along the bore. It covers the design, mounting, and operation of the probe, along with the calibration procedure to determine the field and to prepare a field map for GEANT4 analysis. Additionally, the paper addresses the challenges of accurately measuring low magnetic fields.

Ghoshal, Probir K. [Thomas Jefferson National Acce↗

Probing individual single atom electrocatalyst sites by advanced analytical scanning transmission electron microscopy

Single atom electrocatalysts (SAEs) are promising next-generation materials for promoting a variety of important reactions, such as the oxygen reduction, nitrogen reduction, and CO 2 reduction reactions. While bulk characterization techniques such as X-ray absorption spectroscopy and Mössbauer spectroscopy have significantly enhanced our understanding of these catalysts, direct probing of individual single metal atom sites at the atomic scale is necessary to understand local variations in the properties of these sites and accelerate design and synthesis of improved SAEs. Aberration-corrected scanning transmission electron microscopy (STEM) has become a powerful tool for providing this type of atomic-scale information about SAE metal sites. These sites are typically unstable under the electron beam, however, which, in combination with conventional acquisition methods and detectors, has limited the type and quantity of information obtainable by spectroscopic STEM techniques. Here, we map multiple individual SAE metal sites in a nitrogen-doped carbon containing atomically dispersed Fe and Re (FeReNC) at the atomic scale by direct electron detection electron energy-loss spectroscopy (EELS). Direct electron detection provides an improved signal-to-noise ratio over conventional scintillator-based detectors and enables detection and real space localization of weak signals. In addition, we demonstrate an automated method for identification of metal atom positions, placement of the probe on these sites, and simultaneous EELS and energy dispersive X-ray spectroscopic (EDS) signal acquisition. This simultaneous acquisition of EELS and EDS provides access to the composition and bonding of a wide range of SAE metal sites. In this study, focusing the probe directly on the metal sites also increases the relevant data acquisition rate by more than an order of magnitude over two-dimensional mapping, enabling improved statistical measurements of site properties. The versatility, sensitivity, and speed that these techniques provide enhances our ability to probe the local elemental and chemical environment of a large number of individual SAE metal site structures at the atomic scale, enabling an improved understanding of the variations in the local properties of these electrocatalysts to be gained. As a result, significantly increased information about individual metal sites will be available to future electrochemical studies through these techniques, accelerating the development of advanced SAEs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale decoupling of electronic nematicity and structural anisotropy in FeSe thin films

In a material prone to a nematic instability, anisotropic strain in principle provides a preferred symmetry-breaking direction for the electronic nematic state to follow. This is consistent with experimental observations, where electronic nematicity and structural anisotropy typically appear hand-in-hand. In this work, we discover that electronic nematicity can be locally decoupled from the underlying structural anisotropy in strain-engineered iron-selenide (FeSe) thin films. We use heteroepitaxial molecular beam epitaxy to grow FeSe with a nanoscale network of modulations that give rise to spatially varying strain. We map local anisotropic strain by analyzing scanning tunneling microscopy topographs, and visualize electronic nematic domains from concomitant spectroscopic maps. While the domains form so that the energy of nemato-elastic coupling is minimized, we observe distinct regions where electronic nematic ordering fails to flip direction, even though the underlying structural anisotropy is locally reversed. The findings point towards a nanometer-scale stiffness of the nematic order parameter.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Investigations of Polymethacrylate Tribochemical Films Using X-Ray Spectroscopy and Optical Profilometry

This study investigates the elemental composition and surface morphology of solid tribochemical films formed on steel surfaces. The reversible addition-fragmentation chain transfer (RAFT) method was used to synthesize nine different metal-free polymers, which were blended into commercial base oils. The polymers were either homopolymers of dodecyl methacrylate and ethylhexyl methacrylate or were co-polymers of these monomers with six polar monomers. After tribological testing at 100 degrees C using the ball-on-flat geometry, the resulting tribochemical films were imaged using scanning electron microscopy (SEM) and optical microscopy. The resulting tribochemical films have thicknesses around 50-100 nm. Two of the films corresponding to small (P1-imidazole-containing copolymer) and large (P3-less polar homopolymer) wear were cross-sectioned using focused ion beam (FIB) and analyzed for elemental composition using energy-dispersive X-Ray (EDX) mapping. Oxygen and nitrogen enrichment was observed, consistent with the relative chemical composition of the precursor polymers. Transmission electron microscopy (TEM) evidence suggests that at the worn surface, some organic elements penetrate or are mixed into the steel substrate giving an interlocking appearance. The two samples examined with TEM showed that P1 tribofilm is diffused or mixed with the steel substrate more so than P3, suggesting a stronger affinity and contact during tribofilm formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Design and commissioning of an e-beam irradiation beamline at the Upgraded Injector Test Facility at Jefferson Lab

We report the Upgraded Injector Test Facility (UITF) at Jefferson Lab is a continuous-wave superconducting linear accelerator capable of providing an electron beam with energy up to 10 MeV. A beamline for electron-beam irradiation has been designed, installed and successfully commissioned at this facility, aimed at the degradation study of 1,4-dioxane and per- and polyfluoroalkyl substances (PFAS) in wastewater treatment. A solenoid with a peak axial magnetic field of up to 0.28 T and a set of raster coils were used to obtain a Gaussian beam profile with a transverse standard deviation of ~ 15.0 mm at the target location. Monte-Carlo simulations using FLUKA were carried out to calculate the total absorbed dose and the dose distribution in the sample volume inside the target cell. The simulations were benchmarked experimentally by dosimetry mapping using optichromic dosimeters. The results of the irradiation experiments showed a ~ 95% reduction of 1,4-dioxane in ultra-pure water for a dose of 1 kGy, demonstrating the potential of electron-beam irradiation towards addressing growing challenges in environmental remediation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Structural Complexities in Sodium Ion Conductive Antiperovskite Revealed by Cryogenic Transmission Electron Microscopy

Here we use low-dose cryogenic transmission electron microscopy (cryo-TEM) to investigate the atomic-scale structure of antiperovskite Na 2 NH 2 BH 4 crystals by preserving the room-temperature cubic phase and carefully monitoring the electron dose. Via quantitative analysis of electron beam damage using selected area electron diffraction, we find cryogenic imaging provides 6-fold improvement in beam stability for this solid electrolyte. Cryo-TEM images obtained from flat crystals revealed the presence of a new, long-range-ordered supercell with a cubic phase. The supercell exhibits doubled unit cell dimensions of 9.4 Å × 9.4 Å as compared to the cubic lattice structure revealed by X-ray crystallography of 4.7 Å × 4.7 Å. The comparison between the experimental image and simulated potential map indicates the origin of the supercell is a vacancy ordering of sodium atoms. This work demonstrates the potential of using cryo-TEM imaging to study the atomic-scale structure of air- and electron-beam-sensitive antiperovskite-type solid electrolytes.

36 MATERIALS SCIENCE↗

Development and Use of an Ultra-High Resolution Electron Scattering Apparatus

In this LDRD project, we developed a versatile capability for high-resolution measurements of electron scattering processes in gas-phase molecules, such as ionization, dissociation, and electron attachment/detachment. This apparatus is designed to advance fundamental understanding of these processes and to inform predictions of plasmas associated with applications such as plasma-assisted combustion, neutron generation, re-entry vehicles, and arcing that are critical to national security. We use innovative coupling of electron-generation and electron-imaging techniques that leverages Sandia’s expertise in ion/electron imaging methods. Velocity map imaging provides a measure of the kinetic energies of electrons or ion products from electron scattering in an atomic or molecular beam. We designed, constructed, and tested the apparatus. Tests include dissociative electron attachment to O2 and SO2, as well as a new method for studying laser-initiated plasmas. This capability sets the stage for new studies in dynamics of electron scattering processes, including scattering from excited-state atoms and molecules.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗