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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 613 records · Page 34
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The ORNL Moderator Test Station Science Case

Oak Ridge National Laboratory (ORNL) hosts two world-leading slow neutron sources, the Spallation Neutron Source (SNS) and the High Flux Isotope Reactor (HFIR), and is currently developing the technical design for a Second Target Station (STS) for the SNS. Upon completion of the STS project, ORNL will be uniquely positioned to optimize each of its three neutron sources, the SNS First Target Station (FTS), the STS, and HFIR, in a complementary way. Among the essential aspects of a re-imagined FTS and the current STS design are high-brightness parahydrogen moderators—moderators which are optimized for high per-unit-area neutron brightness rather than integrated-across-large-area neutron intensity. The high-brightness moderators proposed for the STS will, for the brightness metric, significantly outperform the coupled moderators currently on the FTS for appropriately optimized neutron beamlines, provided the moderating hydrogen is converted to near-equilibrium levels of parahydrogen (approximately 99.8% at 20 K). The original FTS moderators, by contrast, were conservatively designed to be relatively insensitive to the exact ortho:para ratio, with a consequent loss in performance. As a result, a redesign of the FTS moderators assuming fully converted parahydrogen could result in significant performance improvements on the FTS coupled moderators, and more consistent performance over time for all hydrogen moderators. This “parahydrogen problem” is a long-standing challenge for the effective implementation of hydrogen cold moderators at high-power neutron sources. In addition, the development of new moderator concepts, whether based on previously unused materials, structured heterogeneous arrays, or even simply on changes in overall shape and size is significantly restricted at a large-scale production facility intended to use the resulting neutron beams. Accordingly, moderators for production neutron sources are often designed in a very conservative, low-risk fashion, even though this compromises the absolute neutronic performance. Advanced moderator concepts worthy of study include features that could not be tested without redesigning and redeploying the entire existing reflector, shielding, and neutron beamline installation, making such development efforts far more expensive than building a stand-alone test facility.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2025

Bayesian model mixing with multireference energy density functional

Reliably predicting nuclear properties across the entire chart of isotopes is important for applications ranging from nuclear astrophysics to superheavy science to nuclear technology. To this day, however, all the theoretical models that can scale at the level of the chart of isotopes remain semiphenomenological. Because they are fitted locally, their predictive power can vary significantly; different versions of the same theory provide different predictions. Bayesian model mixing takes advantage of such imperfect models to build a local mixture of a set of models to make improved predictions. Earlier attempts to use Bayesian model mixing for mass table calculations relied on models treated at single-reference energy density functional level, which fail to capture some of the correlations caused by configuration mixing or the restoration of broken symmetries. In this study we have applied Bayesian model mixing techniques within a multireference energy density functional (MR-EDF) framework. We considered predictions of two-particle separation energies from particle number projection or angular momentum projection with four different energy density functionals—a total of eight different MR-EDF models. We used a hierarchical Bayesian stacking framework with a Dirichlet prior distribution over weights together with an inverse log-ratio transform to enable positive correlations between different models. We found that Bayesian model mixing provides significantly improved predictions compared to the participating models. Published by the American Physical Society 2025

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Role of low-lying resonances for the 10 Be(p,α) 7 Li reaction rate and implications for the formation of the Solar System

Evidence for the presence of short-lived radioactive isotopes when the Solar System formed is preserved in meteorites, providing insights into the conditions at the birth of our Sun. A low-mass core-collapse supernova had been postulated as a candidate for the origin of 10Be, reinforcing the idea that a supernova triggered the formation of the Solar System. We present a detailed study of the production of 10Be by the ν process in supernovae, which is very sensitive to the reaction rate of the major destruction channel, 10 Be(p,α) 7 Li. With data from recent nuclear experiments that show the presence of a resonant state in 11B at ≈193 keV, we derive new values for the 1 0 Be(p,α) 7 Li reaction rate, which are significantly higher than previous estimates. We show that, with the new 10 Be(p,α) 7 Li reaction rate, a low-mass CCSN is unlikely to produce enough 10 Be to explain the observed 10 Be/ 9 Be ratio in meteorites, even for a wide range of neutrino spectra considered in our models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Deciphering the Mechanism of Base-Triggered Conversion of Ammonia to Molecular Nitrogen and Methylamine to Cyanide

Here we report an in-depth investigation into the ammonia oxidation mechanism by the catalyst [Ru III (tpy)(dmabpy)NH 3 ] 3 + ([Ru(NH 3 )] 3 + ). Stoichiometric reactions of [Ru(NH 3 )] 3 + were carried out with exogenous noncoordinating bases to trigger a proposed redox disproportionation reaction, which was followed using variable-temperature NMR spectroscopy. An intermediate species was identified as a dinitrogen-bridged complex using 15 N NMR and Raman spectroscopy on isotopically labeled complexes. This intermediate is proposed to derive from coupling of nitridyl species formed upon sequential redox disproportion reactions. Acetonitrile displaces the dinitrogen bridge to yield free N 2 . DFT calculations support this lower-energy pathway versus that previously reported for ammonia oxidation by the parent [Ru III (tpy)(bpy)NH 3 ] 3 + complex. These experimental and computational results are consistent with the interpretation of redox disproportionation involving sequential hydrogen atom transfer reactions by an amide/aminyl intermediate, [Ru(NH 2 ) – ] + $\Leftrightarrow$ [Ru(NH 2 ) • ] + , formed upon deprotonation of the parent complex. Control experiments employing a large excess of ammonia as a base indicate this new proposed lower-energy pathway contributes to the oxidation of ammonia to dinitrogen in conditions relevant to electrocatalysis. In addition, analogous methylamine complexes, [Ru(NH 2 CH 3 )] 2 + /3 + , were prepared to further test the proposed mechanism. Treating [Ru(NH 2 CH 3 )] 3 + with a base cleanly yields two products [Ru(NH 2 CH 3 )] 2 + and [Ru(CN)] + in an ~3:1 ratio, fully consistent with the proposed cascade of hydrogen atom transfer reactions by an intermediate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Dynamical Avenues for Mercury’s Origin. I. The Lone Survivor of a Primordial Generation of Short-period Protoplanets

The absence of planets interior to Mercury continues to puzzle terrestrial-planet formation models, particularly when contrasted with the relatively high derived occurrence rates of short-period planets around Sun-like stars. Recent work proposed that the majority of systems hosting hot super-Earths attain their orbital architectures through an epoch of dynamical instability after forming in quasi-stable, tightly packed configurations. Isotopic evidence seems to suggest that the formation of objects in the super-Earth-mass regime is unlikely to have occurred in the solar system as the terrestrial-forming disk is thought to have been significantly mass deprived starting around 2 Myr after the formation of calcium-aluminum-rich inclusions—a consequence of either Jupiter’s growth or an intrinsic disk feature. Nevertheless, terrestrial-planet formation models and high-resolution investigations of planetesimal dynamics in the gas-disk phase occasionally find that quasi-stable protoplanets with mass comparable to that of Mars emerge in the vicinity of Mercury’s modern orbit. In this paper, we investigate whether it is possible for a primordial configuration of such objects to be cataclysmically destroyed in a manner that leaves Mercury behind as the sole survivor without disturbing the other terrestrial worlds. We use numerical simulations to show that this scenario is plausible. In many cases, the surviving Mercury analog experiences a series of erosive impacts, thereby boosting its Fe/Si ratio. A caveat of our proposed genesis scenario for Mercury is that Venus typically experiences at least one late giant impact.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Constraining Inputs to Realistic Kilonova Simulations through Comparison to Observed r -process Abundances

Kilonovae, one source of electromagnetic emission associated with neutron star mergers, are powered by the decay of radioactive isotopes in the neutron-rich merger ejecta. Models for kilonova emission consistent with the electromagnetic counterpart to GW170817 predict characteristic abundance patterns, determined by the relative balance of different types of material in the outflow. Assuming that the observed source is prototypical, this inferred abundance pattern in turn must match r -process abundances deduced by other means, such as what is observed in the solar system. We report on analysis comparing the input mass-weighted elemental compositions adopted in our radiative transfer simulations to the mass fractions of elements in the Sun, as a practical prototype for the potentially universal abundance signature from neutron star mergers. We characterize the extent to which our parameter inference results depend on our assumed composition for the dynamical and wind ejecta and examine how the new results compare to previous work. We find that a dynamical ejecta composition calculated using the FRDM2012 nuclear mass and FRLDM fission models with extremely neutron-rich ejecta ($Y_e$ = 0.035) along with moderately neutron-rich ($Y_e$ = 0.27) wind ejecta composition yields a wind-to-dynamical mass ratio of $M_w$/$M_d$ = 0.47, which best matches the observed AT2017gfo kilonova light curves while also producing the bestmatching abundance of neutron capture elements in the solar system, though, allowing for systematics, the ratio may be as high as of order unity.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

High-Current Light-Ion Cyclotron for Applications in Nuclear Security and Radioisotope Production

In this article, we propose the conceptual design, with supporting beam dynamics results, of a normal conducting, separated-sector cyclotron with a strong-focusing field gradient designed to accelerate light ions with a charge-to-mass ratio of 1/2 up to 15–20 MeV/u. The design can support a host of applications for therapy, radiobiology, material science, and instrumentation development. The light-ion species, which can include a mixed ion beam, can be dynamically chosen to provide a range of characteristic signals appropriate for specific material identification such as special nuclear materials. A conservative baseline concept is presented which has been optimized for radioisotope production of alpha emitters and theranostic radiopharmaceuticals. The modular design is also demonstrated to be scalable in gross physical parameters by a factor of 2–3, thereby reducing the size, weight, and power requirements (SWaP) and enabling near-term security applications.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

US EPA Superfund Radon Vapor Intrusion Screening Level (RVISL) Electronic Calculator - 20340

Currently, there is no U.S. Environmental Protection Agency (EPA) guidance on correlating soil or groundwater levels of radon with indoor radon concentrations at Superfund sites. EPA is developing the Radon Vapor Intrusion Level Calculator (RVISL) Calculator which is an online tool. The RVISL calculator: (1) lists three radon isotopes (Rn-219, Rn-220 and Rn-222) known to pose a potential cancer risk through the inhalation pathway; (2) provides generally recommended risk and Applicable or Relevant and Appropriate Requirements (ARAR) based preliminary remediation goals (PRG) for groundwater, soil gas (exterior to buildings and sub-slab) and indoor air for default target risk and ARAR based levels and exposure scenarios; and (3) allows calculation of site-specific PRGs based on user-defined target risk and ARAR based levels and exposure scenarios. EPA developed the RVISL calculator to help risk assessors, remedial project managers, and others involved with risk assessment and decision making at radioactively contaminated sites. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

The Cost of (In-) Accurate Waste Characterization in the U.S. Nuclear Power Industry - 20066

Proper disposal of waste has never been a human priority. Our history is full of examples of throwing away things with minimal effort or thought to consequence. That is until disease or toxicity become apparent and we realize we need to change. Unfortunately, we almost never have all the information we need at the time we make decisions. In addition to the technical and scientific issues, profits and politics are also factors. Newton's third law also applies to politics and so for every policy (action) put in place, there will be (opposite reaction) forces in play to push back against it. These forces are seldom balanced and so the reaction to the discovery of harm is to over-correct and destroy the benefit to be had. This of course causes those who want the benefit, or profit from it, to work to undermine or repeal those measures put in place to eliminate the harm. The issue is exacerbated when the problem to be solved is highly technical and at the edge of our science so that the harm and benefit cannot be easily or accurately quantified. At these times, reason often goes out the window and our decision makers are influenced by either greed or fear as these emotions are much easier to stoke. Those of us in the middle, with the charge to 'do the right thing for the least cost', are therefore frequently constrained and forced into actions that are neither technically the right thing to do and not cost effective. The cost of radioactive waste disposal is based on the concentrations of various radioisotopes in the waste. Some of these isotopes are relatively easy to quantify and some are not. Most laboratory methods for quantification are limited in the amount of activity that can be present during the measurement process. Current nuclear plants were not designed with the idea that taking truly representative waste samples would be important. The limits used to define waste class and therefore cost are precisely defined but the methods for determining those concentrations are far less precise. Improving the accuracy of radioactivity concentrations in waste and having consistent and reasonable oversight can reduce waste costs through active management of the process. So what can we do about it? Science may provide an answer. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Fast switching magnet for heavy ion beam separation

This paper presents the design for a switching magnet capable of deflecting 6.5 MeV/u heavy-ion beams with mass-to-charge ratio of 7 by 10 degrees. This magnet can produce variable flat-top pulses from 1 to 30 ms with rise and fall times of less than 0.5 ms at a variable duty cycle of 3–91% into a heavily inductive load. The magnet has a laminated, iron dominated, H-shaped core. Directly-cooled copper pancake coils energize the magnet. We present the magnet design considerations, including the results of extensive computer modeling. Finally, we also present the conceptual engineering design and the studies of magnet yoke fabrication.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Green's function knockout formalism

Knockout nuclear reactions, in which a nucleon is removed from a nucleus as a result of the collision with another nucleus, have been widely used as an experimental tool, both to populate isotopes further removed from stability and to obtain information about the single-particle nature of the nuclear spectrum. In order to fully exploit the experimental information, theory is needed for the description of both the structure of the nuclei involved, and the dynamics associated with the nucleon removal mechanisms. Here, the standard approach, using theoretical shell-model spectroscopic factors for the structure description coupled with an eikonal model of reaction, has been successful when used in the context of the removal of valence nucleons in nuclei close to stability. However, it has been argued that the reaction theory might need to be revisited in the case of exotic nuclei, more specifically for highly asymmetric nuclei in which the deficient species (neutrons or protons) is being removed. We present here a new formalism for the nucleon-removal and -addition reaction through knockout and transfer reactions, that treats consistently structure and reaction properties using dispersive optical potentials. In particular, our formalism includes the dynamical effects associated with the removal of a nucleon from the projectile, which might explain the long standing puzzle of the quenching of spectroscopic factors in nuclei with extreme neutrons-to-protons ratios.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Statistical chronometry of Meteorites: II. Initial abundances and homogeneity of short-lived radionuclides

Astrophysical models of planet formation require accurate radiometric dating of meteoritic components by short-lived (Al-Mg, Mn-Cr, Hf-W) and long-lived (U-Pb) chronometers, to develop a timeline of such events in the solar nebula as formation of Ca-rich, Al-rich Inclusions (CAIs), chondrules, planetesimals, etc. CAIs formed mostly around a time (“t=0”) when the short-lived radionuclide 26 Al (t 1/2 = 0.72 Myr) was present and presumably homogeneously distributed at a known level we define as ( 26 Al/ 27 Al) SS = 5.23 × 10 -5 . The time of formation after t=0 of another object can be found by determining its initial ( 26 Al/ 27 Al) 0 ratio and comparing it to ( 26 Al/ 27 Al) SS . Dating of meteoritic objects using the Mn-Cr or Hf-W systems is hindered because the abundances ( 53 Mn/ 55 Mn) SS and ( 182 Hf/ 180 Hf) SS at t=0 are not known precisely. To constrain these quantities, we compile literature Al-Mg, Mn-Cr, Hf-W and Pb-Pb data for 13 achondrites and use novel statistical techniques to minimize the discrepancies between their times of formation across these systems. We find that for ( 53 Mn/ 55 Mn) SS = (7.80±0.36)×10 -6 , ( 182 Hf/ 180 Hf) SS = (10.41 ± 0.12) × 10-5, t SS = 4568.65 ± 0.10 Myr, and a 53 Mn half-life of 3.98 ± 0.22 Myr, these four free parameters make concordant 18 formation times recorded by the different systems in all six known volcanic achondrites (the quenched angrites D’Orbigny, Sahara 99555, Northwest Africa 1670; the psuedo-eucrites Asuka 881394 and Ibitira; and the basaltic achondrite Northwest Africa 7325). These parameters also make concordant the ages derived for chondrules from CB/CH achondrites, formed simultaneously in an impact. The other seven achondrites are not quite concordant, but are plutonic angrites or ‘carbonaceous achondrites’ for which simultaneous closure of the isotopic systems might not be expected. Our findings provide very strong support for homogeneity of 26 Al, 53 Mn, and 182 Hf in the solar nebula, and our approach offers a path for more precise chronometry

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Measurement of the $\textit{B}(\textit{E}2 ↑)$ strengths of 36 Ca and 38 Ca

In this work, the $B(E2, 0^+_1 → 2^+_1)$ strengths of 36 Ca and 38 Ca are measured to be 131(20) $e^2\text{fm}^4$ and 101(11) $e^2\text{fm}^4$, respectively. The $\textit{B}(\textit{E}2)$ value for 36 Ca required a measurement of the p/γ branching ratio because the 2 + state is proton unbound. This branching ratio is $B_p$=0.087(8). These $\textit{B}(\textit{E}2)$ and branching-ratio values can be reproduced in the shell-model with the ZMB2 interaction, an interaction that predicts the $\textit{Z} = 20 \textit{sd}$-shell closure is incomplete with large proton pf-shell occupancies in the ground state. These occupancies are at odds with other shell-model and energy-density-functional calculations of 36 Ca. New data are used to provide an update on constraints of the density dependence of the symmetry energy through mirror charge-radii differences as well as to help reduce uncertainties of the astrophysical important 35 K(p,γ) reaction.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Measurement of 227 Ac impurity in 225 Ac using decay energy spectroscopy

225 Ac is a valuable medical radionuclide for targeted $\alpha$ therapy, but 227 Ac is an undesirable byproduct of an accelerator-based synthesis method under investigation. Sufficient detector sensitivity is critical for quantifying the trace impurity of 227 Ac, with the 227 Ac/ 225 Ac activity ratio predicted to be approximately 0.15% by end-of-bombardment (EOB). Superconducting transition edge sensor (TES) microcalorimeters offer high resolution energy spectroscopy using the normal-to-superconducting phase transition to measure small changes in temperature. By embedding 225 Ac production samples in a gold foil thermally coupled to a TES microcalorimeter we can measure the decay energies of the radionuclides embedded with high resolution and 100% detection efficiency. This technique, known as decay energy spectroscopy (DES), collapses several peaks from $\alpha$ decays into single Q-value peaks. In practice there are more complex factors in the interpretation of data using DES, which we will discuss in this paper. Using this technique we measured the EOB 227 Ac impurity to be (0.142 ± 0.005)% for a single production sample. This demonstration has shown that DES is a useful tool for quantitative measurements of complicated spectra.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Lifetime measurements of states of S 35 , S 36 , S 37 , and S 38 using the AGATA γ -ray tracking spectrometer

Lifetimes or lifetime limits of a small number of excited states of the sulfur isotopes with mass numbers A = 35 , 36, 37, and 38 have been measured using the differential recoil-distance method. The isotopes of sulfur were populated in binary grazing reactions initiated by a beam of 36 S ions of energy 225 MeV incident on a thin 208 Pb target which was mounted in the Cologne plunger apparatus. The combination of the PRISMA magnetic spectrometer and an early implementation of the AGATA γ-ray tracking array was used to detect γ rays in coincidence with projectile-like nuclear species. Lifetime measurements of populated states were measured within the range from about 1 to 100 ps. The number of states for which lifetime measurements or lifetime limits were possible was limited by statistics. For 35 S, the lifetime was determined for the first 1/2 + state at 1572 keV; the result is compared with a previous published lifetime value. The lifetime of the 3 - state of 36 S at 4193 keV was determined and compared with earlier measurements. No previous lifetime information exists for the (6 + ) state at 6690 keV; a lifetime measurement with large associated error was made in the present work. For 37 S, the states for which lifetime limits were established were those at 646 keV with J π = 3/2 - and at 2776 keV with J π = 11/2 - ; there are no previously published lifetime values for excited states of 37 S. Finally, a lifetime limit was established for the J π =(6 + ) state of 38 S at 3675 keV; no lifetime information exists for this state in the literature. Measured lifetime values were compared with the results of state-of-the-art shell-model calculations based on the PSDPF, SDPF-U, and FSU effective interactions. In addition, nuclear magnetic-dipole and electric-quadrupole moments, branching ratios, mixing ratios, and electromagnetic transition rates, where available, have been compared with shell-model values. The current work suffers from poor statistics; nevertheless, lifetime values and limits have been possible, allowing a useful discussion of the ability of state-of-the-art shell-model calculations to reproduce the experimental results.

electromagnetic transitions↗
DOE OSTI2021

SR19021 Tritium Aging of Regenerated LANA.75 (Final Project Report)

The Savannah River Tritium Enterprise (SRTE) has used the metal hydride LaNi 4.25 Al 0.75 (LANA.75) in the Tritium Facilities for over two decades. LANA.75 beds store significant quantities of tritium but have a limited service life due to the radiolytic decay of tritium to He-3 within the metal matrix. It has been shown that heating tritium-aged LANA.75 under vacuum can reverse tritium aging effects, eliminating the heel of trapped hydrogen, and restoring the reversible capacity. Additional investigation is needed to ensure there are no unexpected changes to the hydride before this restoration technique is employed in full scale beds in the Tritium Facilities. This project was to be comprised of three distinct scopes: obtain tritium aging data on the sample regenerated in 2018, regenerate a tritium-aged sample at 600 °C, and perform thermal stability testing on a non-tritiated sample. Isotherms were collected on the previously regenerated sample after approximately two years of tritium aging. Isotherms were collected at 80, 100, and 120 °C. As expected, there was a decrease in the plateau pressure, an increase in plateau slope, and a portion of the “heel” of tritium trapped in the metal had been reestablished. Unexpectedly, it appeared that the plateau had shortened at the higher tritium to metal ratios as well. This is typically seen in older samples. The second scope, to regenerate a second tritium-aged LANA.75 sample, was not completed. A Task Technical and Quality Assurance Plan was written and approved, a high temperature test cell was fabricated, several pre-job briefs were held, and the hydride sample was passivated with air. Despite these successes, the hydride sample was not recovered from the legacy test cell. The third scope was to perform thermal stability testing on a “cold” LANA.75 sample. A non-tritiated sample of LANA.75 was held at 750 °C under vacuum for 200 hours to simulate exposure to multiple regeneration evolutions. Hydride isotherm performance, chemical composition, crystallinity, particle size, and morphology are compared between the pre- and post-regeneration samples. No significant changes were observed in composition, crystallinity, or particle size. Comparison of before and after isotherms showed that performance improved rather than deteriorated during the evolution. Scanning Electron Microscopy (SEM) analysis showed small growths on the particle surface after exposure to regeneration conditions. Additional testing will be required to determine the cause of these growths.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Selective Detection of Diglycolamide Diastereomers By Metal-Ligand Cluster Formation

Introduction (120 words): Differentiation of isomers using mass spectrometry is a challenge, as these species tend to produce ions of identical mass-to-charge ratio. Therefore, separation with mass spectrometry must rely on chemical differences between isomeric species. Separation of stereoisomers is especially challenging, as these species often have very similar chemistry. However, recent investigations of the solvent extraction behavior of diastereomers of diglycolamide molecules have shown that different stereoisomers can have significantly different lanthanide extraction efficiencies. These studies showed that the R,S stereoisomer of 2,2'-oxybis(N,N-dioctylpropanamide efficiently extracts lanthanides, while the S,S stereoisomer does not. Thus, gas-phase metal complexation may provide a pathway for differentiating these species using mass spectrometry. Methods (120 words): Europium, samarium, and holmium clusters with the R,S, and the S,S diastereomers of 2,2'-oxybis(N,N-didecylpropanamide (trivially tetradecyl diglycolamide, or mTDDGA) were generated in gas-phase using the electrospray ionization source of a Bruker (Billerica, MA, USA) micrOTOF-Q II quadrupole time-of-flight mass spectrometer. Solutions of aqueous lanthanide nitrate and diglycolamide ligands in 2-propanol were added to 50%:50% by volume acetonitrile:2-propanol to generate the spray solutions. Ligand concentration was maintained at approximately 6 µM, while lanthanide concentration was maintained at either 6 µM or 30 µM . High resolution, high mass accuracy spectra were recorded using the time-of-flight. Mass accuracy was ensured using external calibration with Agilent (Santa Clara, CA, USA) ESI-L Low Concentration tuning mix. Preliminary data (300 words): Electrospray of solutions containing only R,S-mTDDGA or S,S-m-TDDGA yield abundant peaks at m/z= 721.7, corresponding to [mTDDGA+H]+1, m/z = 743.7, corresponding to [mTDDGA+Na]+1, and m/z = 1464.4, corresponding to the sodium-bound dimer, [Na(mTDDGA)2]+1. Spray of solutions containing 6 µM europium (Eu) with 3 µM R,S-mTDDGA produced an abundant cluster ion with an isotopic envelope centered at m/z=772.0, corresponding to [Eu(R,S-mTDDGA)3]3+. Europium-containing cluster ions with isotopic envelopes apexing at m/z = 1012.3 and 1189.0 correspond to the [Eu(R,S-mTDDGA)4]3+ and [Eu(R,S-mTDDGA)5]3+ cluster ions, respectively. Protonated and sodiated R,S-mTDDGA are present as well, along with the sodium-bound dimer. In contrast, spray of solutions containing 6 µM europium (Eu) with 3 µM S,S-mTDDGA diastereomer yielded only protonated and sodiated ligand ions; no Eu- S,S-mTDDGA ions were present. This mirrors the solution-phase behavior, where the S,S diestereomer extracts lanthanides with significantly less efficiency than the R,S diestereomer. Experiments with holmium and samarium yielded the same results. Increasing the lanthanide concentration to 30 µM resulted in limited formation of lanthanide-S,S-mTDDGA clusters. However, the abundance of the [Ln(S,S-mTDDGA)3]3+ clusters remained low compared to the abundance of the protonated and sodiated ligand. Additionally, the abundance of the [Ln(R,S-mTDDGA)3]3+ cluster ion was significantly higher than that of the protonated and sodiated ligand in experiments with spray solutions containing 30 µM lanthanide with R,S-mTDDA, supporting the hypothesis that R,S-mTDDGA has a higher intrinsic affinity for the lanthanides than S,S-mTDDGA. Thus, the intrinsic complexation with lanthanides appears to offer a route to differentiate diglycolamide diestereomers in the gas-phase. Novelty (20): Stereoisomers can be differentiated in the gas phase by exploitation of differences in metal complexation chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

The Extent of Solar Energetic Particle Irradiation in the Sun’s Protoplanetary Disk

Solar flares emit X-rays and high-energy (MeV to GeV) ions called solar energetic particles (SEPs). Astronomical observations show solar-mass protostellar fluxes are a factor Φ ≈ 3 × 10 2 –3 × 10 3 times higher than the present-day Sun. Constraining Φ in the early solar system is important for modeling ionization in the Sun’s protoplanetary disk, the extent of magnetorotational instability or magnetocentrifugal outflows, or even production of short-lived radionuclides. Recent interpretations of meteoritic data—including cosmogenic Ne in hibonite grains, initial ( 10 Be/ 9 Be) 0 ratios in Ca-rich, Al-rich inclusions (CAIs), or even inferences of live 7 Be in CAIs—suggest values Φ > 10 5 , reaching as high as Φ ≈ 6 × 10 6 , which would make the young Sun extraordinarily active, even for a protostar. We constrain Φ by reexamining these data. We conclude that cosmogenic Ne was produced in hibonite grains as they resided in the disk; 36 Cl was created in Cl-poor grains after the disk dissipated; 10 Be was inherited from the molecular cloud, with almost no (<1%) 10 Be created in the disk; and there is no evidence whatsoever for any live 7 Be in CAIs. We show these data are consistent with a value Φ ≈ 3 × 10 3 for the first >5 Myr of the solar nebula. The early Sun evidently emitted a flux of X-rays and SEPs not atypical for a protostar.

79 ASTRONOMY AND ASTROPHYSICS↗