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At least 127 records · Page 7

Learning neural representations for X-ray ptychography reconstruction with unknown probes

X-ray ptychography provides exceptional nanoscale resolution and is widely applied in materials science, biology, and nanotechnology. However, its full potential is constrained by the critical challenge of accurately reconstructing images when the illuminating probe is unknown. Conventional iterative methods and deep learning approaches are often suboptimal, particularly under the low-signal conditions inherent to low-dose and high-speed experiments. These limitations compromise reconstruction fidelity and restrict the broader adoption of the technique. In this work, we introduce the Ptychographic Implicit Neural Representation (PtyINR), a self-supervised framework that simultaneously addresses the object- and probe-recovery problem. By parameterizing both as continuous neural representations, PtyINR performs end-to-end reconstruction directly from raw diffraction patterns without requiring any pre-characterization of the probe. Extensive evaluations demonstrate that PtyINR achieves superior reconstruction quality on both simulated and experimental data, with remarkable robustness under challenging low-signal conditions. Furthermore, PtyINR offers a generalizable, physics-informed framework for addressing probe-dependent inverse problems, making it applicable to a wide range of computational microscopy problems.

36 MATERIALS SCIENCE↗

Block copolymer self-assembly derived mesoporous magnetic materials with three-dimensionally (3D) co-continuous gyroid nanostructure

Magnetic nanomaterials are gaining interest for their many applications in technological areas from information science and computing to next-generation quantum energy materials. While magnetic materials have historically been nanostructured through techniques such as lithography and molecular beam epitaxy, there has recently been growing interest in using soft matter self-assembly. In this work, a triblock terpolymer, poly(isoprene-block-styrene-block-ethylene oxide) (ISO), is used as a structure directing agent for aluminosilicate sol nanoparticles and magnetic material precursors to generate organic–inorganic bulk hybrid films with co-continuous morphology. After thermal processing into mesoporous materials, results from a combination of small angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) are consistent with the double gyroid morphology. Nitrogen sorption measurements reveal a type IV isotherm with H1 hysteresis, and yield a specific surface area of around 200 m 2 g −1 and an average pore size of 23 nm. The magnetization of the mesostructured material as a function of applied field shows magnetic hysteresis and coercivity at 300 K and 10 K. Comparison of magnetic measurements between the mesoporous gyroid and an unstructured bulk magnetic material, derived from the identical inorganic precursors, reveals the structured material exhibits a coercivity of 250 Oe, opposed to 148 Oe for the unstructured at 10 K, and presence of remnant magnetic moment not conventionally found in bulk hematite; both of these properties are attributed to the mesostructure. This scalable route to mesoporous magnetic materials with co-continuous morphologies from block copolymer self-assembly may provide a pathway to advanced magnetic nanomaterials with a range of potential applications.

Chemistry↗

Probing molecular wavepacket evolution using multidimensional coherent spectroscopy (Final Report)

The goal of this project was to develop and demonstrate multidimensional coherent spectroscopy (MDCS) techniques to fully map wave-packet dynamics in simple molecules. MDCS correlates excitation and emis sion frequencies, enabling continuous tracking of wave-packet evolution even when multiple wave-packets evolve simultaneously. The initial experiments were to be performed using the MDCS apparatus in the PI’s laboratory to record the evolution of the wave-packet’s energy in molecular iodine. A longer-term goal was to develop a version compatible with using an X-ray Free Electron Laser (XFEL) as a probe, which would allow the evolution of the internuclear distance of the wave-packet—not just its energy—to be determined.

74 ATOMIC AND MOLECULAR PHYSICS↗

Thermal Inspection for the Assessment of Adhesively Bonded Metal Adherends

Certification of adhesively bonded structures is currently a challenge for aircraft manufacturers. The ability to certify bonds in primary structure can reduce dependence on fasteners and this will enable more efficient manufacturing. For example, drilling holes and installing fasteners in bonded joints can be a potentially significant bottleneck in airframe manufacturing. In addition, fasteners increase the airframe weight and can add stress concentration areas. Reducing fastener count can accelerate manufacturing and improve aircraft performance. NASA is currently investigating nondestructive evaluation (NDE) techniques to assess bond integrity. For example, bond thickness influences bond strength and therefore NDE techniques are being investigated to determine bond thickness. For bonded metal structures, there is a large difference in the thermal diffusivity between the 7075 aluminum alloy metal adherends and aircraft grade adhesive. Multi-layered thermal models show a large variation in the thermal response for bondline adhesive thicknesses that vary from 100 to 300 microns for adherend thicknesses of 0.163 cm. Experimental through-transmission thermal measurements reveal promise to quantitatively characterize the bondline thickness. Results were validated with X-ray computed tomography and optical microscopy measurements, and influence of porosity on the thermal model and measurements are investigated.

X-ray computed tomography↗

Thermal Inspection for the Assessment of Adhesively Bonded Metal Adherents

Certification of adhesively bonded structures is currently a challenge for aircraft manufacturers. The ability to certify bonds in primary structure can reduce dependence on fasteners and this will enable more efficient manufacturing. For example, drilling holes and installing fasteners in bonded joints can be a potentially significant bottleneck in airframe manufacturing. In addition, fasteners increase the airframe weight and can add stress concentration areas. Reducing fastener count can accelerate manufacturing and improve aircraft performance. NASA is currently investigating nondestructive evaluation (NDE) techniques to assess bond integrity. For example, bond thickness influences bond strength and therefore NDE techniques are being investigated to determine bond thickness. For bonded metal structures, there is a large difference in the thermal diffusivity between the 7075 aluminum alloy metal adherends and aircraft grade adhesive. Multi-layered thermal models show a large variation in the thermal response for bondline adhesive thicknesses that vary from 100 to 300 microns for adherend thicknesses of 0.163 cm. Experimental through-transmission thermal measurements reveal promise to quantitatively characterize the bondline thickness. Results were validated with X-ray computed tomography and optical microscopy measurements, and influence of porosity on the thermal model and measurements are investigated.

bondline thickness↗

Characterization and effects of impurities on carbonate quantification in heterogenous matrices

Mineral carbonation simulates a natural weathering phenomena by breaking down silicates and oxides to form Ca & Mg carbonates. Various mineralization methods have been demonstrated as a potential technique to improve the quality of slags and tailings through neutralization and stabilization of problematic species to yield a product better suited for use in concrete. This study aims to characterize, quantify and analyze carbonates in various carbonated products such as mineralized CaCO 3 , CO 2 mineralized Steel Slags and Mine Tailings. More than 10 samples were analyzed for carbonate measurement and verification from industrial and academic partners that pioneer commercial CO 2 mineralization technologies. The samples were characterized primarily by using X-ray diffraction (XRD), Thermogravimetric Analyses (TGA), and Scanning Electron Microscopy (SEM) to gain insights into CaCO 3 content. A baseline characterization of lab-grade CaCO 3 and MgCO 3 also revealed important considerations for CaCO 3 measurement using TGA alone. The experiments using synthetic lab-grade samples also revealed that the presence of MgCO 3 /MgO can accelerate the decomposition of CaCO 3 and thus can affect measurement parameters. Lab-grade CaCO 3 samples dosed into steel slag and mine tailing also showed significant deviation in their decomposition behavior. These insights are used to inform the development of a standardized protocol for the measurement and verification of carbonate-bearing products.

97 MATHEMATICS AND COMPUTING↗

Surface science insight note: A linear algebraic approach to elucidate native films on Fe 3 O 4 surface

Standard materials are often used to obtain spectra that can be compared to those from unknown samples. Spectra measured from these known substances are also used as a means of computing sensitivity factors to allow quantification by X-ray photoelectron spectroscopy (XPS) of less well-defined materials. Spectra from known materials also provide line shapes suitable for inclusion in spectral models which, when fitted to spectra, permit the chemical state for a sample to be assessed. Both types of information depend on isolating photoemission signals from the inelastically scattered signal. In this Insight note, technical issues associated with the use of XPS of as received Fe 3 O 4 powder sample surface are discussed. The Insight note is designed to show how linear algebraic techniques applied to data collected from a sample marketed as pure Fe 3 O 4 powder are used to verify that XPS has been performed on chemistry representative of the sample. The methods described in this Insight note can further be utilized in elucidating complex XPS data obtained from thin films formed or evolved during cyclic/non-steady use of complex (electro)catalyst surfaces, especially in the presence of contaminants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast Laser Welding and Terahertz Time-domain Spectroscopy of Soda Lime Silicate Glass

Joining and welding techniques of similar and dissimilar materials have reached their limits due to the inflexibility of adapting dielectric materials, e.g., glasses and ceramics, reproducibility for transparent materials, and cycle process time. The ability to join pieces of glasses using laser irradiation allows rapid processing of vacuum insulating glass (VIG) for a widening range of commercial energy-efficient applications. We have used a 1064-nm laser wavelength with 15 picoseconds pulse width and a 155-kHz repetition rate to weld commercial plate glass pieces. The welded samples were characterized via x-ray fluorescence (XRF), time-of-flight secondary ion mass spectrometry (TOF–SIMS), polarimetry, and terahertz time-domain spectroscopy (THz-TDS) to determine the integrity of the weld and chemical changes in the welded areas. Our data shows no significant changes in glass chemistry and structure on average over nano- to micro-scales occurred from the welding process within the limits of the characterization tools. Our results demonstrate successful welding of glass plates without significant changes in the glass chemistry, structure, or properties in the laser-modified region or strains in the bulk glass.

Matthies, Kathleen [ORNL] (ORCID:0009000213135441)↗

Multiplet lines in seeded stimulated Mn 𝐾⁢𝛼 1 x-ray emission

We report the successful resolution of the multiplet structure of 𝐾⁢𝛼 1 x-ray emission in manganese (Mn) complexes through seeded stimulated x-ray emission spectroscopy (seeded S-XES). Using a femtosecond pump pulse above the Mn 𝐾 edge to generate simultaneous 1⁢𝑠 core holes, and a second-color tunable seed pulse to initiate the stimulated emission process, we were able to enhance individual lines within the 𝐾⁢𝛼 1 emission. This approach allows to resolve the fine multiplet features that are obscured by lifetime broadening in conventional (spontaneous) Mn 𝐾⁢𝛼 XES. The work builds on our previous observation that S-XES from Mn(II) and Mn(VII) complexes pumped at high intensities can exhibit stimulated emission without sacrificing the chemical sensitivity to oxidation states. Furthermore, this technique opens the door to controlled high-resolution electronic structure spectroscopy in transition-metal complexes beyond the core-hole lifetime, with potential applications in catalysis, inorganic chemistry, and materials science.

Chemical Physics & Physical Chemistry↗

Chemical and Radiological Compatibility Testing of 3D Printed Materials

To dramatically increase the adaptability, performance, and safety of processes in support of the Defense Waste Processing Facility (DWPF), Savannah River National Lab (SRNL) plans to perform chemical and radiological compatibility testing on a wide variety of 3D printed materials of interest. The 3D printing process provides numerous strategic operational benefits such as rapid prototyping of complex designs and geometry specific to the needs of the nuclear waste disposition process, as well as on-demand rapid prototyping and iteration with materials that aren’t as accessible through traditional manufacturing methods. Reaction chemistry in simulated waste batches can be matched closely to its radioactive counterpart, but glass reactor vessels have limitations. Vessel geometry can play a big factor in mixing transport limitations, process chemistry, and degradation reaction kinetics. In addition, additive manufacturing allows for much more detailed vessel design than traditional alternatives. Waste processing techniques in DWPF also encounter extreme chemical environments including high pH, strong acids, abrasive slurries, and significant irradiation. To meet these challenges, a matrix of various polymer, ceramic, and metal additive manufacturing materials have been exposed to a suite of chemical environments of interest as well as radioactive dose (such as gamma radiation from 60 Co) to properly test their durability under these conditions. Mass change has been monitored over a period of up to a week in these conditions, as well as added characterization for surface modification through Scanning Electron Microscopy/Electron Dispersive X-ray analysis (SEM/EDX). Further chemical characterization has been monitored through Fourier-Transform InfraRed Spectroscopy (FTIR), with planned investigation via thermal and tensile strength degradation. While the direct product of this research is identification of material(s) that can withstand specific hazardous environments encountered by the mercury water wash tank in DWPF process simulation experiments, the reference base of materials will be used for many other nuclear processes in the pursuit of rapidly developed, cost-efficient, and highly specific devices for environmental remediation and much more.

Wilson, Nathan W. [Savannah River National Laborat↗

Deep learning‑based metal artefact reduction in X-ray computed tomography of TRISO fuel compacts

TRISO (TRi-structural ISOtropic) – compact-type micro-particle fuels – are next generation nuclear fuel compacts designed with safety in mind. Structural integrity and characterisation before and after irradiation are important to determine the performance of the fuel compacts under real reactor conditions. X-ray computed tomography can be an important tool for non-destructive evaluation of these fuel compacts. The fuel particles are highly attenuating for X-rays which creates metal artefact, rendering the images unusable. Our artefact correction can mitigate these artefacts significantly. The proposed method works by first segmenting highly-attenuating structures (metal) and forward projecting to localise the source of artefacts in the projection domain, then, using a traditional or U-net-based deep learning architecture, contextually interpolating those regions to remove the artefacts. Finally the reconstruction from the modified projection is fused with the segmented metal. The proposed method shows a significant improvement in the image quality while significantly reducing the reconstruction time compared to the standard technique.

Rahman, Obaid [ORNL] (ORCID:0000000277810840)↗

Single-particle chemical analysis reveals organic-rich detonation soot products

The detonation of high explosives produces a wide variety of particulate matter (PM) with distinct properties, not all of which are traditionally studied for chemical composition, formation processes, and forensic applications. We report particle-resolved measurements of Composition B detonation soot using soot particle aerosol mass spectrometry (SP-AMS), identifying carbonaceous species and metals not previously characterized on a single-particle basis. Results are combined with scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDS) to enhance source-dependent signatures. Black carbon, including graphitic carbon and detonation nanodiamonds, contributed 50.5-71.4% of PM 2.5 mass, while 22.5-43.4% was non-refractory organic carbon, a previously overlooked component that exhibited a complex and varying composition. Detonations were performed with and without PMMA confinement and under steady and overdriven conditions. Distinct particles enriched with polycyclic aromatic hydrocarbons (PAHs) were observed in experiments utilizing confinement, with quantities dependent on manufacturing method. SEM-EDS validated SP-AMS findings of metals internally mixed with carbonaceous species and extended the particle size range to 100 µm. This work makes detecting non-refractory organics using single-particle techniques more feasible for detonation forensics and understanding high-energy soot formation. While this analysis uses offline sample collection, SP-AMS could be deployed for in-situ measurements of detonation PM 2.5 transported in the atmosphere.

36 MATERIALS SCIENCE↗

Structural and physicochemical insights into pH-responsive poly(DEAEMA- co -HEMA)-grafted mesoporous silica nanoparticles

Mesoporous silica nanoparticles (SiO 2 ) grafted with responsive polymer shells are versatile hybrid systems. Understanding their three-dimensional organization in the hydrated state remains a significant challenge. Here, in this study, SiO 2 nanoparticles were functionalized with a poly(DEAEMA-co-HEMA) shell via a “grafting-from” polymerization strategy in aqueous media. Successful surface modification was confirmed by FTIR, thermogravimetric analysis, transmission electron microscopy, X-ray photoelectron spectroscopy, N 2 sorption, and ζ-potential, yielding grafting contents of 22% (p1 DEAEMA-co-HEMA ) and 49% (p2 DEAEMA-co-HEMA ). Small-angle neutron scattering (SANS) with solvent contrast variation was employed to elucidate the solution-state core–shell architecture of p1 and p2 hybrids at pH 2, where the grafted polymer shell is protonated and highly hydrated. Near contrast matching of the silica core, theoretically estimated at 58% D 2 O, suppressed the scattering intensity, enhancing sensitivity to the polymer shell. Constrained core–shell ellipsoid modeling across solvent contrasts revealed a systematic increase in shell thickness, overall particle dimensions, and shell anisotropy with increasing grafting content. In solution, the hydrated polymer shells were markedly more extended and structurally anisotropic than suggested by dry-state techniques structural characterization, highlighting the importance of solution-state structural analysis for accurately describing grafted polymer architectures.

Core-shell biomaterials↗

Adaptively coupled phase retrieval in multi-peak Bragg coherent diffraction imaging

Recent advances in Bragg coherent diffraction imaging (BCDI) experimental techniques permit routine measurement of multiple Bragg peaks from a single crystalline grain. The resulting images contain the full lattice distortion vector field which can be differentiated to provide lattice strain and rotation. With the advent of fourth-generation synchrotron light sources, such multi-peak datasets are produced at high rates, facilitating the need for rapid phase retrieval of the multiple peaks and subsequent image analysis. Here we describe and demonstrate a new implementation of a coupled phase retrieval technique for multi-peak BCDI which simultaneously treats each Bragg peak of the dataset and produces a three-dimensional image of the crystal's morphology and lattice distortion field. In addition, this method uses the redundant information contained in the various Bragg diffraction patterns to detect and suppress spurious signal appearing on the detector in a subset of the measurements. Compared with manual data editing, adaptive coupling produces a more consistent phase profile in reciprocal space and sharper surfaces in direct space, with no significant difference in computational cost. These improvements reduce the need for manual preprocessing and enable robust high-throughput analysis of multi-peak BCDI data, supporting near-real-time strain microscopy at modern synchrotron facilities.

36 MATERIALS SCIENCE↗

Strong Effect of Nonpolar Solvent Molecular Structure on CdSe Nanoplatelet Stacking

We report a drastic difference in stacking behavior of oleic acid-stabilized 4-monolayer (4 ML) CdSe nanoplatelets (NPLs) in toluene and methylcyclohexane (MCH), two nonpolar solvents that differ in the conformational flexibility of their molecules. Using liquid cell transmission electron microscopy (TEM) and small angle scattering (SAXS) techniques, we show that NPLs form microns-long ribbons consisting of 4 ML CdSe NPLs in toluene, the solvent widely used to form stable colloidal solutions of a broad range of quasi-spherical nanoparticles. In contrast, 4 ML CdSe NPLs are well dispersed in MCH. The difference in stacking behavior of NPLs in toluene and MCH suggests that the conformational flexibility of the solvent molecules, such as the ability to adopt multiple chair conformations, modulates nanoplatelet interactions. Molecular dynamics (MD) simulations reveal that solvent molecules subtly alter the structure of the organic ligand shell. These solvent-dependent changes propagate to the inorganic core, modulating the degree of CdSe nanoplatelet (NPL) twisting and, consequently, the properties of the nanoparticles. We show that toluene better solvates oleate ligands while MCH induces a bimodal oleate span distribution, which can lead to increased solubility of CdSe NPLs. In addition, the solvent can also influence the inorganic core, which, in turn, can modify the nanoparticle properties. We demonstrate that destabilization of toluene solution containing ribbons of 4 ML CdSe NPLs without CdS shells results in the formation of NPL assemblies with amplified spontaneous emission (ASE) with a low threshold of 14 µJ cm−2 that is comparable with that of CdSe/CdS core/shell NPLs. Our results emphasize that the solvent plays a major role in mediating interactions between NPLs and hence their processability for fabrication of functional structures.

CdSe↗

4D insights into lithium-ion battery sidewall rupture during thermal runaway

Thermal runaway (TR), characterized by rapid exothermic reactions, presents a serious safety risk in lithium-ion batteries (LiBs). External triggers such as high temperatures, mechanical abuse, or internal short circuits (ISCs) can initiate TR, often resulting in sidewall rupture, which may escalate to catastrophic battery pack failure. In this study, we developed and applied high-speed synchrotron imaging techniques to investigate sidewall rupture mechanisms in LiBs subjected to different triggering scenarios. Using in situ 4D tomographic imaging, we visualized the dynamic evolution of sidewall rupture with high spatial and temporal resolution. The results revealed distinct failure behaviors linked to each trigger, underscoring the complex and condition-specific nature of sidewall breach and battery failure. These insights highlight the critical importance of implementing tailored safety strategies across diverse applications. Our findings demonstrate the powerful potential of synchrotron high-speed tomography as a diagnostic tool for advanced safety testing and cell qualification.

25 ENERGY STORAGE↗

Full-polarization millimeter wavelength variability of Sagittarius A * during the 2018 EHT campaign

Context. Sagittarius A* (Sgr A*), the supermassive black hole at the center of the Milky Way, provides a unique laboratory to study accretion dynamics and plasma processes near the event horizon. Aims. We investigated the variability and polarization properties of Sgr A* using ALMA observations during the 2018 Event Horizon Telescope campaign. Methods. We analyzed high-cadence full-polarization light curves from ALMA at millimeter wavelengths, performed time-series analysis, and investigated the temporal behavior during an X-ray flare observed by Chandra on 2018 April 24. The variability characteristics are compared with expectations from standard accretion flow models. Results. We find low variability in total intensity (σ/μ < 10%), but significantly higher variability in linear and circular polarization (∼30% and ∼50%, respectively). A time-series analysis reveals red-noise variability, with power spectral densities between −2 and −3 across all Stokes parameters. Polarized intensity shows stable intra-day timescales, while total intensity exhibits more variable timescales, suggesting distinct emission regions, with polarization likely arising from a coherent structure. On April 24, a statistically significant inter-band delay in polarized intensity coincides with a near-simultaneous X-ray and millimeter peak that deviates from the typical delayed flare scenario. This event also features enhanced millimeter variability and coherent polarization loop evolution. The observed simultaneity challenges standard models of transient synchrotron emission with cooling delays, favoring instead a scenario of continuous energy injection in an optically thin region. Conclusions. Our results offer new constraints on the physical mechanisms driving variability in Sgr A*, and provide key observational input for refining theoretical models of accretion and plasma behavior in the vicinity of supermassive black holes.

Galaxy: center↗

Surface Reordering During Layer‐by‐Layer Growth on SrTiO 3

With the development of layer‐by‐layer growth techniques such as molecular beam epitaxy (MBE), it is now possible to construct materials with atomic‐level precision, with the layer sequence primarily determined by the growth recipe. However, materials can still restructure in the high‐temperature growth environment with surface thermodynamics strongly influencing growth behavior. Here, we demonstrate that growth on ${\rm SrTiO}_{3}$ (001), the principal platform for oxide electronics, does not occur in a layer‐by‐layer fashion but follows a more complex process in which a ${\rm TiO}_{2}$ plane continually diffuses toward the growth surface. Employing in situ synchrotron X‐ray scattering combined with ab initio thermodynamic calculations, we discover the existence of a stable ${\rm TiO}_{2}$ double‐layer structure on the pristine substrate and the occurrence of dynamic layer rearrangement during homoepitaxial growth by oxide MBE. Our findings suggest that the current methods used to precisely control ${\rm SrTiO}_{3}$ surfaces are limited, as well as our ability to dictate the composition of ultrathin films, resulting in important ramifications regarding the surface reactivity of perovskite materials grown on ${\rm SrTiO}_{3}$.

Coherent Bragg Rod Analysis↗