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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 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Production of High Specific Activity 155 Tb, 161 Tb and 203 Pb for Research and Clinical Applications: Effective Target Design, Target Material Recycling and Radioisotope Separation (Final Technical Report)

The overall objectives of this project were (1) to develop methods for the production and separation of a diagnostic and therapeutic or “theranostic” pair of radioisotopes, terbium-155 ( 155 Tb) and terbium-161 ( 161 Tb) and (2) to train graduate students and postdoctoral fellows in technologies and methods used in radionuclide production. Radionuclides can be incorporated into drugs called radiopharmaceuticals that target a specific disease (e.g., cancer). The need for theranostic radionuclides is escalating with the clinical translation of radiopharmaceuticals due to their implementation in personalized medicine, which has demonstrated enhanced patient treatments. High purity and high specific activity radionuclides are critical for theranostic agent development, for example to maintain diagnostic image quality, to minimize radiation dose to the patient, and to increase uptake in the targeted tissue (e.g., tumor), especially in the case of receptor- and antigen-targeted agents. The 155 Tb (diagnostic) and 161 Tb (therapeutic) radioisotopes that were generated through this project are a theranostic pair with demonstrated potential for the development and translation into individualized, targeted, and dosimetry-driven radiotherapies. However, the development of such radiotherapies has been hindered by the lack of a routine and reliable supply of these isotopes in the United States. Methods for the production, separation, and supply of 155 Tb and 161 Tb were investigated and developed in this project. Further, the strong emphasis throughout the project on the training of graduate students and postdoctoral fellows has helped to ensure and enhance the nuclear science workforce through the training of the next generation of highly qualified scientists in nuclear and radiochemistry. This grant also continued a collaboration between scientists at the University of Washington (UW), the University of Missouri (MU) and Brookhaven National Laboratory (BNL). All three institutions were involved in the project, but to different degrees on the various tasks through which the overall objectives were met.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Photonuclear cross sections for the 197 Au ⁢(𝛾, 𝑝⁢𝑛)⁢ 195⁢𝑚 Pt reaction near threshold

Platinum radioisotopes are of growing interest for targeted cancer therapy and diagnostic imaging because their decay delivers highly localized radiation doses in tissue, herewith enabling precise DNA damage through Auger-electron emission. Developing production technologies that provide platinum isotopes with high specific activity is essential in radioisotope therapy. Photonuclear reactions on stable nuclei offer a viable accelerator-based route for isotope production when supported by reliable cross-section data. We report photonuclear cross-section measurements for the 197 Au(γ, pn) 195m Pt reaction at incident γ-ray energies of 27, 29, and 31 MeV using the activation method. The measurements were performed by irradiating a stack of concentric-ring gold targets with a quasi-monoenergetic γ-ray beam provided by the High Intensity Gamma-ray Source (HI γS). The induced 195m Pt activity was quantified using off-line γ-ray spectroscopy. These data provide the first experimental constraints on the 197 Au(γ, pn) 195m Pt cross section in the near-threshold region. Furthermore, the comparison of the measured excitation function to PHITS and TALYS calculations indicates that the reaction becomes measurable only near 30 MeV and that substantially higher bremsstrahlung end-point energies are required for practically meaningful production.

190 ≤ A ≤ 219↗
DOE OSTI2025

Non–linear bonding trends in maleonitrile-1,2–dithiolate complexes of the transuranium actinides

The trivalent actinides are produced in the nuclear fuel cycle during power production and provide the largest long-term radiation dose in used nuclear fuel. It is ideal for these elements to be removed from used nuclear fuel for disposal and a necessity for fuel recycling. A key challenge to this is the similarity of chemical behavior of the trivalent actinides to the lanthanides that are also present as fission products in used fuel. Thus far, some of the most effective separations of actinides from lanthanides utilise chelating agents containing sulfur moieties such as dithiophosphinates that selectively bind to actinide ions because of a greater bond covalency relative to lanthanide ions. Typically, greater differences between actinide and lanthanide ions are observable the more ligands and chelators bonds have a covalent character. Here, a series of complexes of the trivalent actinides Np(III) through Cf(III) (excluding Bk(III)) with maleonitrile-1,2-dithiolate (mnt 2– ) are synthesized along with their lanthanide counterparts (La(III) – Nd(III), Sm(III) – Gd(III), Dy(III)), in order to characterize the nature of chemical bonds with these metal ions and a polarizable, non-innocent, sulfur-donor ligand. The metal-sulfur bonds in these complexes trend shorter than measured for lanthanides with equivalent ionic radii. However, particularly large deviations are observed in the neptunium and plutonium complexes in both structure and bonding, resulting in a nonlinear bond length trendline for the actinide series. Density Functional Theory (DFT) calculations with Quantum Theory of Atoms in Molecules (QTAIM) and Natural Bond Order (NBO) analyses indicate that for the neptunium and plutonium complexes, the presence of increased 5f-orbital participation, energy degeneracy of the metal and ligand orbitals, and the structure packing result in shortened M–S bonds. The stabilization of the energy of the 5f-orbitals and the decrease in f-contribution to bonding orbitals in the later actinides results in structural properties more similar to the lanthanide complexes.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

An exploration of benchtop X–ray emission spectroscopy for precise characterization of the sulfur redox state in cementitious materials

The evolution of sulfur chemistry in cements is best known in the bailiwick of failure mechanisms via sulfate attack but is equally important for its contributions to the reduction capacity of cementitious materials often used for immobilizing nuclear waste streams destined for long-term storage, e.g., cementitious waste forms (CWF). The total reduction capacity of CWFs, encompassing contributions from both S and Fe reductants, and its implications toward radionuclide immobilization is most often studied by destructive wet chemistry methods requiring acid digestion in the presence of Ce(IV) and subsequent titration and colorimetric interpretation. Here, we investigate a similarly analytical but nondestructive alternative, benchtop high resolution wavelength-dispersive x-ray fluorescence spectroscopy, most commonly known as x-ray emission spectroscopy (XES), for probing the bulk sulfur oxidation state distribution. We present here an initial investigation of S XES, including an improved experimental protocol for lab XES of inhomogeneous samples, both as a complement to the Ce(IV) test and for new scientific opportunities that it enables for observing changes in sulfur chemistry. We discuss future improvements and opportunities, including: (1) the practical challenges associated with coordinating XES and Ce(IV) liquid extraction for a more comprehensive perspective on reduction capacity and for a high-precision evaluation of uncertainties in the Ce(IV) test; and (2) new opportunities, due to the nondestructive nature of XES, for controlled evolution studies aimed at elucidating specific chemical responses of CWF’s exposed to invasive gas or liquid species or to accelerated aging by radiative dose or thermal treatment.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Optimizing Treatment in Intermediate-Risk Prostate Cancer: Secondary Analysis of a Randomized Phase 3 Trial

To identify patients with intermediate-risk prostate cancer (IRPC) benefiting from de-escalation of androgen deprivation therapy (ADT) and/or dose escalated radiation therapy (DERT), we performed a secondary analysis of a phase 3 trial by measuring biochemical failure (BF), distant metastases, prostate cancer–specific mortality, overall survival (OS), and distant metastases-free survival (DMFS) rates according to prognostic intermediate risk factors (IRF).

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2026

High energy X-ray characterization of the microstructure of PuGa alloy samples at macroscopic depths and non-ambient conditions

High energy (95 keV) X-rays were utilized to characterize the microstructure of eight PuGa alloy samples at room temperature and during cooling to ∼10 K. The samples had different Ga content (nominally 0-3.4 at.%), age, and history. A ninth sample, similarly characterized with neutron diffraction, was included to extend the Ga range to 7 at.%. The samples span the range from single phase α (monoclinic) to δ (face-centered cubic) PuGa, as well as a two-phase α′/δ sample. The crystallographic textures, phase fractions, lattice parameters and dislocation densities of each sample were evaluated through distinct analysis techniques. The textures of the samples were modest. In each case, the dislocation densities were relatively high, comparable to cold worked metals and metals exposed to similar radiation dose. At room temperature, the lattice parameters determined in the predominantly single-phase samples were larger than expected based on the nominal Ga concentration. The observed lattice thermal expansions of the single-phase δ samples to 10 K are self-consistent across the samples and consistent with previous measurements reported in the literature. Significantly larger thermal lattice strain is observed in the δ phase of the two-phase material due to mechanical constraint from the α′ phase, which has a three times larger thermal expansion and is much harder than the δ phase. In conclusion, the results demonstrate the unique value of high-energy X-rays for relatively routine microstructural characterization of Pu alloy samples.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Pulse Radiolysis Investigation of Radicals Derived from Water-Soluble Cyanine Dyes: Implications for Super-resolution Microscopy

Light-induced blinking, an inherent feature of many forms of super-resolution microscopy, has been linked to transient reduction of the fluorescent cyanine dye used as an imaging agent. There is, however, only scant literature information related to one-electron reduced cyanine dyes, especially in an aqueous environment. Here, we examine a small series of cyanine dyes, possessing disparate π-conjugation lengths, under selective reducing or oxidizing conditions. The experiment allows recording of both differential absorption spectra and decay kinetics of the resultant one-electron reduced or oxidized transient species in water. Relative to the ground state, absorption transitions for the various radicals are weak and somewhat broadened but do allow correlation with the π-conjugation length. In all cases, absorption maxima lie to the blue of the main ground-state transition. Under anaerobic conditions, the transient species decay on the microsecond to millisecond time scale, with the mean lifetime depending on molecular structure, radiation dose, and dye concentration. The experimental absorption spectra recorded for the one-electron reduced radicals and the presumed dimer cation radical compare well to spectra obtained from time-dependent density functional theory calculations. Furthermore, the results allow conclusions to be drawn regarding the plausibility of the reduced species being responsible for light-induced blinking in direct stochastic optical reconstruction microscopy.

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

Spin Solar Cell Phenomenon on a Single-Molecule Magnet (SMM) Impacted CoFeB-Based Magnetic Tunnel Junctions

The single-molecule magnet (SMM) is demonstrated here to transform conventional magnetic tunnel junctions (MTJs), a memory device used in present-day computers, into solar cells. For the first time, we demonstrated an electronic spin-dependent solar cell effect on an SMM-transformed MTJ under illumination from unpolarized white light. We patterned cross-junction-shaped devices to form a CoFeB/MgO/CoFeB-based MTJ. The MgO barrier thickness at the intersection between the two exposed junction edges was less than the SMM extent, which enabled the SMM molecules to serve as channels to conduct spin-dependent transport. The SMM channels yielded a region of long-range magnetic ordering around these engineered molecular junctions. Our SMM possessed a hexanuclear [Mn 6 (μ 3 -O) 2 (H 2 N-sao) 6 (6-atha) 2 (EtOH) 6 ] [H 2 N-saoH = salicylamidoxime, 6-atha = 6-acetylthiohexanoate] complex and thioesters end groups to form bonds with metal films. SMM-doped MTJs were shown to exhibit a solar cell effect and yielded ≈80 mV open-circuit voltage and ≈10 mA/cm 2 saturation current density under illumination from one sun equivalent radiation dose. A room-temperature Kelvin Probe AFM (KPAFM) study provided direct evidence that the SMM transformed the electronic properties of the MTJ’s electrodes over a lateral area in excess of several thousand times larger in extent than the area spanned by the molecular junctions themselves. As a result, the decisive factor in observing this spin-photovoltaic effect is the formation of SMM spin channels between the two different ferromagnetic electrodes, which in turn is able to catalyze the long-range transformation in each electrode around the junction area.

14 SOLAR ENERGY↗
DOE OSTI2023

Ultra-short pulse laser acceleration of protons to 80 MeV from cryogenic hydrogen jets tailored to near-critical density

Laser plasma-based particle accelerators attract great interest in fields where conventional accelerators reach limits based on size, cost or beam parameters. Despite the fact that particle in cell simulations have predicted several advantageous ion acceleration schemes, laser accelerators have not yet reached their full potential in producing simultaneous high-radiation doses at high particle energies. The most stringent limitation is the lack of a suitable high-repetition rate target that also provides a high degree of control of the plasma conditions required to access these advanced regimes. Here, we demonstrate that the interaction of petawatt-class laser pulses with a pre-formed micrometer-sized cryogenic hydrogen jet plasma overcomes these limitations enabling tailored density scans from the solid to the underdense regime. Our proof-of-concept experiment demonstrates that the near-critical plasma density profile produces proton energies of up to 80 MeV. Based on hydrodynamic and three-dimensional particle in cell simulations, transition between different acceleration schemes are shown, suggesting enhanced proton acceleration at the relativistic transparency front for the optimal case.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Ion irradiation induced phase transformation in gold nanocrystalline films

Gold is a noble metal typically stable as a solid in a face-centered cubic (FCC) structure under ambient conditions; however, under particular circumstances aberrant allotropes have been synthesized. In this work, we document the phase transformation of 25 nm thick nanocrystalline (NC) free-standing gold thin-film via in situ ion irradiation studied using atomic-resolution transmission electron microscopy (TEM). Utilizing precession electron diffraction (PED) techniques, crystallographic orientation and the radiation-induced relative strains were measured and furthermore used to determine that a combination of surface and radiation-induced strains lead to an FCC to hexagonal close packed (HCP) crystallographic phase transformation upon a 10 dpa radiation dose of Au 4+ ions. Contrary to previous studies, HCP phase in nanostructures of gold was stabilized and did not transform back to FCC due to a combination of size effects and defects imparted by damage cascades.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Accurate real space iterative reconstruction (RESIRE) algorithm for tomography

Tomography has made a revolutionary impact on the physical, biological and medical sciences. The mathematical foundation of tomography is to reconstruct a three-dimensional (3D) object from a set of two-dimensional (2D) projections. As the number of projections that can be measured from a sample is usually limited by the tolerable radiation dose and/or the geometric constraint on the tilt range, a main challenge in tomography is to achieve the best possible 3D reconstruction from a limited number of projections with noise. Over the years, a number of tomographic reconstruction methods have been developed including direct inversion, real-space, and Fourier-based iterative algorithms. Here, we report the development of a real-space iterative reconstruction (RESIRE) algorithm for accurate tomographic reconstruction. RESIRE iterates between the update of a reconstructed 3D object and the measured projections using a forward and back projection step. The forward projection step is implemented by the Fourier slice theorem or the Radon transform, and the back projection step by a linear transformation. Our numerical and experimental results demonstrate that RESIRE performs more accurate 3D reconstructions than other existing tomographic algorithms, when there are a limited number of projections with noise. Furthermore, RESIRE can be used to reconstruct the 3D structure of extended objects as demonstrated by the determination of the 3D atomic structure of an amorphous Ta thin film. We expect that RESIRE can be widely employed in the tomography applications in different fields. Finally, to make the method accessible to the general user community, the MATLAB source code of RESIRE and all the simulated and experimental data are available at https://zenodo.org/record/7273314.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Advancing X-ray quantum imaging through Monte-Carlo simulations

Imaging with X-rays poses fundamental limits due to radiation damage of the highly energetic photons. This becomes problematic for sensitive biological systems such as subcellular structures. Lowering the radiation dose, without sacrificing the signal-to-noise ratio, would be desirable for any kind of imaging modalities involving X-rays. To achieve this goal, quantum imaging with entangled X-ray photons constitutes a promising route. Production of biphotons have been demonstrated in the X-ray regime by the process of Spontaneous Parametric Down-Conversion (SPDC). However, compared to SPDC in the regime of visible light, the production rate for X-ray biphotons is extremely low. With the introduction of new high average brightness X-ray sources, such as 4th generation synchrotrons and high repetition rate Free-Electron X-ray Lasers (XFEL), quantum imaging may become practical. We introduce a ray tracing approach using Monte-Carlo sampling, specifically designed for quantum imaging with entangled X-ray photons generated by SPDC. By simulation, the superior image quality of quantum over classical imaging methods is demonstrated using realistic experimental conditions available at high repetition rate XFELs. With these simulations, we can efficiently assist the design of future experiments at beam lines, which can substantially accelerate the advancement of X-ray quantum imaging and reduce costs.

Entangled Photons↗
DOE OSTI2021

Direct visualization of radiation-induced transformations at alkali halide–air interfaces

Radiation driven reactions at mineral/air interfaces are important to the chemistry of the atmosphere, but experimental constraints (e.g. simultaneous irradiation, in situ observation, and environmental control) leave process understanding incomplete. Using a custom atomic force microscope equipped with an integrated X-ray source, transformation of potassium bromide surfaces to potassium nitrate by air radiolysis species was followed directly in situ at the nanoscale. Radiolysis initiates dynamic step edge dissolution, surface composition evolution, and ultimately nucleation and heteroepitaxial growth of potassium nitrate crystallites mediated by surface diffusion at rates controlled by adsorbed water. Finally, in contrast to in situ electron microscopy and synchrotron-based imaging techniques where high radiation doses are intrinsic, our approach illustrates the value of decoupling irradiation and the basis of observation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Novel dual-reflection design applied for ITER core x-ray spectrometer

Here. a novel dual-reflection configuration is introduced for the International Tokamak Experimental Reactor (ITER) core x-ray spectrometer to fit the allocated space where it will be placed accompanied by moving the detectors backward to reduce the incident radiation dose. The highly oriented pyrolytic graphite, which has a mosaic structure of microscopic crystallites, is chosen for the front reflector motivated by higher x-ray throughput and stronger misalignment tolerance compared to the perfect crystal reflector. In the ITER core x-ray spectrometer, a combination of several reflector-deflected Lines of Sight (LOSs) and a direct LOS is proposed for the first time named X-Ray Crystal Spectroscopy Core (XRCS-Core). The system is optimized to observe lines from externally seeded xenon and the intrinsic tungsten impurity, meeting both port integration needs and measurement requirements. Its spectral performance is simulated using an analytical-raytracing mixed code——XRSA, showing good imaging quality with a spectral resolution higher than 8000. The XRCS-Core system is thought to be applicable in various ITER scenarios through the assessment taking into account the spectrometers’ specifications and the chosen lines’ emissivity in different plasma parameters.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Fiber-optic bolometers with high-temperature tolerance and reduced time constants for fusion plasma diagnostics

Fiber-optic bolometers (FOBs) designed for plasma radiation measurement in magnetically confined fusion environments have been previously developed and tested at the DIII-D tokamak. These FOBs utilize a silicon Fabry–Perot interferometer at the fiber tip for temperature measurement and a gold disk as a radiation absorber. This paper presents recent advancements in the development of FOBs with reduced cooling time constants and enhanced temperature tolerance. We also demonstrate high-temperature operation and report findings from irradiation tests. By incorporating a copper sensor holder as a thermal sink and integrating two closely packed sensor heads into a compact design, the cooling time constants were reduced to ∼100 ms in vacuum, while minimizing uncertainties caused by temperature gradients. The FOBs were subjected to heating at 400 °C for five hours, with no observed degradation in noise performance post-heating. High-temperature operation tests were conducted at ∼220 °C using a 404 nm square-wave modulated laser to simulate the plasma radiation. In addition, four FOBs constructed from copper-coated pure-silica fibers were fabricated and underwent irradiation testing, enduring a total γ-radiation dose of 15.2 MGy and a neutron fluence of 1.6 × 10 18 n/cm 2 . As a result, the FOBs maintained their physical integrity and the optical signal shows high visibility throughout the test.

42 ENGINEERING↗