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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
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The melt memory effects in polymer crystallization

This paper presents a systematic review of the literature on the melt memory effects observed in polymers, an area that has engendered considerable debate for over 50 years. Recent advances in experimental techniques have provided fresh insights into how a polymer's thermal history influences its recrystallization behavior. It has been observed that given other conditions unchanged, the crystallization temperature during recrystallization decreases with an increase in the melt temperature T s above the melting point T m until a critical melt temperature is attained. This phenomenon also extends to the half-time of crystallization and the secondary structures, such as lamellar thickness, of semi-crystalline polymers. Despite these findings, a comprehensive constitutive model that encapsulates polymer melt memory effects remains elusive. Cutting-edge instrumentation, including in situ small and wide-angle X-ray scattering, temperature-controlled Fourier transform infrared spectroscopy, and flash differential scanning calorimetry, have posed significant challenges to the traditional nucleation and growth models established in the 1970s. These models are foundational to our understanding of polymer crystallization, which is an integral part of polymer processing and production. In this review, the historical contours of this discourse are traced, with an examination of both the recent experimental breakthroughs and theoretical advancements pertinent to polymer melt memory effects. In conclusion, this paper delves into the prevailing theories of polymer nucleation and crystallization and engages with theoretical discussions and numerical simulations that attempt to elucidate and rationalize these melt memory phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Early age hydration behavior of portland cement-based binders incorporating fly ash contaminated with flue gas desulfurization products

Fly ash co-mingled with flue gas desulfurization (FGD) products are currently discarded as off-specification materials based on their high SO3 content. However, previous studies have shown that performance of these fly ashes varies significantly based on FGD product type and as such they may be viable for use in low-CO2 concrete as supplementary cementitious materials (SCMs). In this study, fly ashes with three different types of FGD products including calcium sulfite hemihydrate, calcium sulfate (with some unreacted lime), and sodium sulfate (with some unreacted sodium carbonate) were evaluated. The early age hydration behavior in blended cementitious systems at 20% cement replacement level was studied using Vicat setting time tests, isothermal calorimetry, in-situ quantitative X-ray diffraction, and pore solution analysis. The cause of the setting time retardation and flash setting observed in fly ashes with calcium sulfite hemihydrate and sodium carbonate, respectively, were identified and suitable beneficiation options were suggested for the valorized use of these materials in low-CO 2 concrete.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Spectral Hardness of X- and Gamma-Ray Emissions From Lightning Stepped and Dart Leaders

During the 2022 New Mexico monsoon season, we deployed two X-ray scintillation detectors, coupled with a 180 MHz data acquisition system to detect X-rays from natural lightning at the Langmuir Lab mountain-top facility, located at 3.3 km above mean sea level. Data acquisition was triggered by an electric field antenna calibrated to pick up lightning within a few km of the X-ray detectors. We report the energies of over 240 individual photons, ranging between 13 keV and 3.8 MeV, as registered by the LaBr3(Ce) scintillation detector. These detections were associated with four lightning flashes. Particularly, four-stepped leaders and seven dart leaders produced energetic radiation. Importantly, the reported photon energies allowed us to confirm that the X-ray energy distribution of natural stepped and dart leaders follows a power-law distribution with an exponent ranging between 1.09 and 1.96, with stepped leaders having a harder spectrum. Characterization of the associated leaders and return strokes was done with four different electric field sensing antennas, which can measure a wide range of time scales, from the static storm field to the fast change associated with dart leaders.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Characterization of Aluminum Metal Powders for Plutonium-238 Program

As part of radioisotope thermoelectric generator (RTG) production for power sources in deep space exploration, Oak Ridge National Laboratory (ORNL) produces plutonium-238 ( 238 Pu). To produce 238 Pu, neptunium-237 ( 237 Np) targets are fabricated at ORNL and subsequently irradiated at the High Flux Isotope Reactor (HFIR) at ORNL and the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Specifically, current flowsheets utilize neptunium dioxide ( 237 NpO 2 ) targets. Aluminum (Al) powder is blended with 237 NpO 2 target material to improve thermal conductivity during irradiation. The current composition of 237 NpO 2 /Al pellets (i.e., cermets, or ceramic–metallics) is 20% 237 NpO 2 , 70% Al, and 10% void space. Al powders utilized by the 238 Pu program are high-fired under vacuum before blending into targets. The primary objective of this work is to measure the physical, chemical, and thermal properties of Al before and after the high-firing process. Properties of interest include the morphology, surface texture, particle size, crystal phase(s), and thermal conductivity of the material. These properties are measured with existing materials characterization equipment at ORNL, including powder x-ray diffraction (pXRD), scanning electron microscopy (SEM) with energy-dispersive spectroscopy (EDS), laser flash analysis (LFA), and thermogravimetric analysis (TGA). A secondary objective of this work is to compare the Al powders before and after the high-firing procedure to determine the effects of high-firing on chemical, physical, and thermal properties and to determine the efficacy of the high-firing process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Flash Communication: Boron K-edge XAS and TDDFT Studies of Covalent Metal–Ligand Bonding in Ni(C 2 B 9 H 11 ) 2

Ligand K-edge X-ray absorption spectroscopy (XAS), a technique that can measure variations in covalent metal–ligand bonding, has rarely been used to assess covalency in complexes containing metal–boron bonds. Here we describe ligand K-edge XAS and TDDFT studies of the Ni dicarbollide complex Ni(C 2 B 9 H 11 ) 2 (1) and the Ni-free salt (HNMe 3 )(C 2 B 9 H 12 ) (L1). The XAS spectrum for 1 reveals a pre-edge feature indicative of covalent Ni–B bonding, which is corroborated by time-dependent density functional theory (TDDFT) calculations and comparative analysis to L1 and inner-shell electron energy loss spectroscopy (ISEELS) collected on the same Ni complex.

Boron↗
DOE OSTI2023

Observation of laser ablation of silicon as a function of pulse length at constant fluence via time-resolved x-ray spectroscopy

We investigate the ablation of silicon as a function of laser pulse length at a constant fluence using time-resolved x-ray spectroscopy data obtained from OMEGA EP experiments at the University of Rochester's Laboratory for Laser Energetics. Our targets consisted of three-layer planar structures composed of Si (50 μm), Cu (25 μm), and SiO 2 (500 μm) layers. The Si layer was irradiated by a 351-nm laser with varying pulse widths of 250 ps, 500 ps, 1 ns, and 10 ns while maintaining a constant fluence of ~27.9 kJ/cm 2 . Electron temperatures and densities of the ablated plasma were determined by analyzing the time-resolved x-ray spectroscopy data through a comparison of experimental measurements with synthetic results obtained from Si atomic calculations in a steady state and non-local thermodynamic equilibrium. These calculations were computed using PrismSPECT. Additionally, radiation-hydrodynamics simulations with FLASH are used to generate simulated plasma-density and plasma-temperature profiles, which are then compared with the experimental measurements. Our analyses reveal that increasing the laser pulse length at a constant fluence results in a decrease in electron temperatures and densities. Furthermore, the longer pulses with lower intensities lead to deeper ablation regions before reaching the peak ablation but lower ionization balances in the silicon layer. Furthermore, these findings emphasize the critical role of laser pulse length in plasma ablation and shock generation for laser-impulse studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Comparison of the photochemical properties of phthalocyanine and hemiporphyrazine Zn(II) complexes

In DMF (dimethylformamide) solutions containing concentrations of (NEt 4 )Br (Et = ethyl) between 0.001 and 0.05 M both zinc phthalocyanine (Pc) and hemiporphyrazine (Hp) complexes are dissolved and form species [Zn(Hp)(Br)] – , and [Zn(Pc)(Br)] – . The increase in formation of the hemiporphyrazine bromide adduct is revealed by a linear dependence of the UV–Vis absorption spectrum on the Br – concentration whereas, over the same concentration range, absorption measurements indicate the formation of the phthalocyanine bromide adduct in solution. The x-ray and molecular structure of [NEt 4 ][Zn(Pc)(Br)](H 2 O) 0.33 has been determined showing the coordination of the Br – to the metal center. Photo-induced processes of the Zn complexes were investigated with deaerated solutions in a time scale t ≥10 ns. The 355 nm flash irradiation of [Zn(Hp)(Br)] – produced transient spectra which showed a bathochromic shift of the absorption maximum from 460 nm to 440 nm and an increase of the spectrum rate of decay with increasing Br – concentrations. The initial spectrum is attributed to the (nπ*–LLCT Br→Hp )[Zn(Hp)(Br)] – excited state which reacts with H-atom donors forming a radical [Zn(Hp-H)(Br)] •– . On the other hand, a transient spectrum, λ max ~600 nm, grows in a time t ≤0.6 µs when [Zn(Pc)(Br)] – is flash irradiated at 355 nm. The photoreactions of these complexes with SCN – and 2-propanol (IPA) were studied. Despite of the apparent similarity between both complexes, IPA was photo-oxidized by both complexes although by different mechanisms, an electron transfer with [Zn(Pc)(Br)] – and an H atom abstraction with [Zn(Hp)(Br)] – . Finally, the photo-oxidation of SCN– by [Zn(Pc)(Br)] – but not by [Zn(Hp)(Br)] – makes a remarkable difference between the photochemistries of these complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

The dynamics, mixing, and thermonuclear burn of compressed foams with varied gas fills

Inertial confinement fusion (ICF) implosions involve highly coupled physics and complex hydrodynamics that are challenging to model computationally. Due to the sensitivity of such implosions to small features, detailed simulations require accurate accounting of the geometry and dimensionality of the initial conditions, including capsule defects and engineering features such as fill tubes used to insert gas into the capsule, yet this is computationally prohibitive. It is therefore difficult to evaluate whether discrepancies between the simulation and experiment arise from inadequate fidelity to the capsule geometry and drive conditions, uncertainties in physical data used by simulations, or inadequate physics. We present results from detailed high-resolution three-dimensional simulations of ICF implosions performed as part of the MARBLE campaign on the National Ignition Facility [Albright et al., Phys. Plasmas 29, 022702 (2022)]. These experiments are foam-filled separated-reactant experiments, where deuterons reside in the foam and tritons reside in the capsule gas fill and deuterium–tritium (DT) fusion reactions only occur in the presence of mixing between these materials. Material mixing in these experiments is primarily seeded by shock interaction with the complex geometry of the foam and gas fill, which induces the Richtmyer–Meshkov instability. We compare results for experiments with two different gas fills (ArT and HT), which lead to significant differences in the hydrodynamic and thermodynamic developments of the materials in the implosion. Our simulation results show generally good agreement with experiments and demonstrate a substantial impact of hydrodynamic flows on measured ion temperatures. The results suggest that viscosity, which was not included in our simulations, is the most important unmodeled physics and qualitatively explains the few discrepancies between the simulation and experiment. The results also suggest that the hydrodynamic treatment of shocks is inadequate to predict the heating and yield produced during shock flash, when the shock converges at the center of the implosion. Alternatively, underestimation of the level of radiative preheat from the shock front could explain many of the differences between the experiment and simulation. Nevertheless, simulations are able to reproduce many experimental observables within the level of experimental reproducibility, including most yields, time-resolved X-ray self-emission images, and an increase in burn-weighted ion temperature and neutron down-scattered ratio in the line of sight that includes a jet seeded by the glue spot that joins capsule hemispheres.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Flash Communication: Flexibility of a Biologically Inspired Ligand Framework for Intramolecular C–H Activation

High-valent iron complexes play a crucial role in the oxidation of organic substrates, especially in C–H bond functionalization reactions in biology. This paper investigates the reactivity of nonporphyrin tripodal ligands featuring a secondary coordination sphere, focusing on their prospective ability to stabilize high-valent iron-oxo species. Using NMR spectroscopy and X-ray crystallography, we detail the formation of an Fe(III)-alkoxide complex through intramolecular C–H bond activation, providing insight into the potential transient formation of a high-valent iron-oxo intermediate. While attempts to observe an Fe(IV)-oxo complex were unsuccessful, our findings underscore the significance of the ligand electronic environment in stabilizing reactive iron species for C–H bond activation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

A Novel Platform for Evaluating Dose Rate Effects on Oxidative Damage to Peptides: Toward a High-Throughput Method to Characterize the Mechanisms Underlying the FLASH Effect

High dose rate radiation has gained considerable interest recently as a possible avenue for increasing the therapeutic window in cancer radiation treatment. The sparing of healthy tissue at high dose rates relative to conventional dose rates, while maintaining tumor control, has been termed the FLASH effect. Although the effect has been validated in animal models using multiple radiation sources, it is not yet well understood. Here, in this work, we demonstrate a new experimental platform for quantifying oxidative damage to protein sidechains in solution as a function of radiation dose rate and oxygen availability using liquid chromatography mass spectrometry. Using this reductionist approach, we show that for both X-ray and electron sources, isolated peptides in solution are oxidatively modified to different extents as a function of both dose rate and oxygen availability. Our method provides an experimental platform for exploring the parameter space of the dose rate effect on oxidative changes to proteins in solution.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2023

A unified non-equilibrium phase change model for injection flow modeling

The homogenous relaxation model (HRM) is one of the most widely used models to describe the liquid- gas phase transition. However, in its original formulation, it is unable to handle multispecies vapor-liquid equilibrium (VLE), which limits its applicability to single-component fluids. In this work, a unified non-equilibrium phase change model that considers the VLE of multicomponent mixtures is proposed building upon the HRM's structure. A time factor is introduced to mimic the effect of different phase change timescales due to different mechanisms, e.g., cavitation, flash-boiling, and evaporation. Here to assess the model's performance, computational fluid dynamics simulations of the internal and near-nozzle injection flow of the Engine Combustion Network's Spray G injector were performed using the nine-component PACE-20 fuel with both the unified model and the original HRM. The predicted fuel density in the near-nozzle region matched well with X-ray tomography measurements. The simulation results indicated that, whereas the HRM failed to capture the vaporization due to convective mixing between the fuel and ambient gas, the unified model performed well in predicting the mixing-driven vaporization and the corresponding evaporative cooling. Further comparisons using the nine-component fuel formula and a single-component fuel surrogate demonstrated the unified model's ability to predict preferential vaporization, which affects the predictions of local mixture composition and rate of vaporization. Finally, it is shown that the unified model is capable of representing multiple phase change mechanisms, and the relaxation time factor plays an important role in determining the degree of phase change due to the different mechanisms.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2023

Flash NanoPrecipitation as an Agrochemical Nanocarrier Formulation Platform: Phloem Uptake and Translocation after Foliar Administration

The increasing severity of pathogenic and environmental stressors that negatively affect plant health has led to interest in developing next-generation agrochemical delivery systems capable of precisely transporting active agents to specific sites within plants. In this work, we adapt Flash NanoPrecipitation (FNP), a scalable nanocarrier (NC) formulation technology used in the pharmaceutical industry, to prepare organic core–shell NCs and study their efficacy as foliar or root delivery vehicles. NCs ranging in diameter from 55 to 200 nm, with surface zeta potentials from -40 to +40 mV, and with seven different shell material properties were prepared and studied. Shell materials included synthetic polymers poly(acrylic acid), poly(ethylene glycol), and poly(2-(dimethylamino)ethyl methacrylate), naturally occurring compounds fish gelatin and soybean lecithin, and semisynthetic hydroxypropyl methylcellulose acetate succinate (HPMCAS). NC cores contained a gadolinium tracer for tracking by mass spectrometry, a fluorescent dye for tracking by confocal microscopy, and model hydrophobic compounds (alpha tocopherol acetate and polystyrene) that could be replaced by agrochemical payloads in subsequent applications. After foliar application onto tomato plants with Silwet L-77 surfactant, internalization efficiencies of up to 85% and NC translocation efficiencies of up to 32% were observed. Significant NC trafficking to the stem and roots suggests a high degree of phloem loading for some of these formulations. Results were corroborated by confocal microscopy and synchrotron X-ray fluorescence mapping. NCs stabilized by cellulosic HPMCAS exhibited the highest degree of translocation, followed by formulations with a significant surface charge. The results from this work indicate that biocompatible materials like HPMCAS are promising agrochemical delivery vehicles in an industrially viable pharmaceutical nanoformulation process (FNP) and shed light on the optimal properties of organic NCs for efficient foliar uptake, translocation, and delivery.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Staged Z-pinch experiment at the double-EAGLE pulsed power facility

The staged Z-pinch is a potential high-energy gain fusion concept where a high atomic number liner implodes on a deuterium target using a pulsed multi-MA current source. Over the past several years this concept has been studied on 0.5–1.0 MA facilities using Ar and Kr gas puffs injected at R = 1.2 cm. Neutron yield up to (2.5 ± 0.34) x 10 10 was measured, Ruskov et al (2023 IEEE Trans. Plasma Sci. 51 3310–6). Here, in this study, we present experimental results from the 4 MA, 110 ns current rise time Double-EAGLE facility at L3Harris (currently, Fisica Inc.) where a larger radius nozzle created gas density profiles peaked at R = 2.5 cm. Modeling with the MACH2 and FLASH codes indicates that the larger radius allows stronger acceleration of the liner plasma and generation of shock waves that preheat a target plasma layer next to the liner to temperatures $T_i >$1 keV. The resulting counter thermal pressure on the liner plasma limits the growth of the Magneto-Rayleigh–Taylor (MRT) instability at the liner-vacuum boundary and the implosion proceeds in a relatively stable manner. Near bang time the enormous target plasma thermal pressure smoothens the MRT perturbations developed during the earlier implosion stages. Time integrated x-ray pinhole images with cutoff energy of 100 eV confirm that a long (∼3 cm), stable and uniform high energy density plasma column is formed in the final implosion stage. Consistent neutron yield in the 10 10 –10 11 range was measured for both Ar and Kr liners imploding on a deuterium target.

Physics - Plasma physics↗
DOE OSTI2023

Volatile propellant droplet evaporation measurements in metered dose inhaler sprays

Many aerosol products rely on the rapid vaporization of volatile propellants to produce a fine spray. In the simplest case, these are binary mixtures of propellant and a delivered product which undergo a flash-evaporation process leaving only the less volatile product in the resultant droplet. In more complex applications, such as pressurized metered-dose inhalers, the non-propellant component may contain dissolved or suspended drug which precipitates or dries to form a matured particle. The size and morphology of the particles depend strongly on the time-history of the droplet as the propellant evaporates. However, measuring the dynamic evaporation processes that occur in dense sprays containing millions of droplets is challenging. In this paper, we demonstrate a novel application of Ultra Small Angle X-ray Scattering to measure the bulk composition of volatile HFC134a–ethanol sprays and compare the obtained results with simple evaporation models in a dry nitrogen environment. The data reveal that diffusion-limiting processes inside the droplet are equally important as external convection and mixing-limited factors in determining evaporative timescales.

42 ENGINEERING↗
DOE OSTI2026

Redirection and reshaping of intense extreme-ultraviolet radiation

The goal to control short-wavelength radiation for the investigation and manipulation of ultrafast dynamics in quantum systems coevolves with the growing availability of extreme-ultraviolet (XUV) and x-ray sources from high-harmonic generation and free-electron lasers. Here, we present an XUV spatio-spectral phase modulator based on an intense XUV laser beam propagating through an optically thick resonant target, introducing dispersion profile variations around the resonance both perpendicular to and along the laser propagation direction. The resulting dipole radiation gets spectrally reshaped and becomes more divergent as compared to the original beam in the far field. As an experimental demonstration, the intense-XUV–induced double-peak off-axis structure in the far-field spectrum obtained at the Free-Electron Laser in Hamburg (FLASH) shows indications of the underlying XUV-driven Rabi dynamics and resonant pulse propagation effects. The presented work highlights a ubiquitous phenomenon occurring when an intense laser beam passes through a resonant medium.

He, Yu [Max-Planck-Institut für Kernphysik, Heidel↗
DOE OSTI2024

Local structure effects of carbon-doping on the phase change material Ge 2 Sb 2 Te 5

Ge 2 Sb 2 Te 5 is used in phase change memory, a nonvolatile memory technology, due to its phase change properties. The primary advantage of phase change memory over the state-of-the-art (flash memory) is its simple and small device geometry, which allows for denser nodes and lower power consumption. In phase change memory, resistive heating induces fast switching between the high resistance amorphous and low resistance crystalline phases, corresponding to storage of low and high digital states, respectively. However, the instability of the amorphous phase of Ge 2 Sb 2 Te 5 presents issues with processing and long-term data storage; such issues can be resolved by C doping, which stabilizes the amorphous phase and raises the crystallization temperature. To better understand the local structural effects of C doping on Ge 2 Sb 2 Te 5 , in situ Ge K-edge X-ray absorption spectroscopy measurements were taken during heating of films with various C doping concentrations. Here, the range of structural transformation temperatures derived from X-ray absorption near-edge structure analysis across the C doping series proved narrower than crystallization temperatures reported in similar in situ X-ray diffraction experiments, which may reflect changes in local structure that precede long-range ordering during crystallization. In addition, rigorous extended X-ray absorption fine structure fitting across and between temperature series revealed effects of C doping on the rigidity of Ge–Te bonds at low (2 at% and 4 at%) C concentrations.

Langhout, John D.↗
DOE OSTI2024

Conditional guided generative diffusion for particle accelerator beam diagnostics

Abstract Advanced accelerator-based light sources such as free electron lasers (FEL) accelerate highly relativistic electron beams to generate incredibly short (10s of femtoseconds) coherent flashes of light for dynamic imaging, whose brightness exceeds that of traditional synchrotron-based light sources by orders of magnitude. FEL operation requires precise control of the shape and energy of the extremely short electron bunches whose characteristics directly translate into the properties of the produced light. Control of short intense beams is difficult due to beam characteristics drifting with time and complex collective effects such as space charge and coherent synchrotron radiation. Detailed diagnostics of beam properties are therefore essential for precise beam control. Such measurements typically rely on a destructive approach based on a combination of a transverse deflecting resonant cavity followed by a dipole magnet in order to measure a beam’s 2D time vs energy longitudinal phase-space distribution. In this paper, we develop a non-invasive virtual diagnostic of an electron beam’s longitudinal phase space at megapixel resolution (1024 × 1024) based on a generative conditional diffusion model. We demonstrate the model’s generative ability on experimental data from the European X-ray FEL.

43 PARTICLE ACCELERATORS↗