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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

2025 ASMS Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS

Title (20 words): Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS Introduction (120 words): One of the challenges facing wide-spread adoption of nuclear power is the development of efficient separation processes for used nuclear fuel. The molecules in separation processes are subjected to an extreme environment due to the high radiation fields from the used fuel and highly acidic media used for fuel dissolution, which results in significant molecular degradation, leading to reduced process efficiency. These degradation products must be identified and studied so mitigation strategies can be developed to maintain process efficiency. However, complex systems can have many degradation products, complicating identification. Untargeted analysis tools could be used to understand radiation chemistry in complex systems. However, this would necessitate improved understanding of the gas-phase fragmentation mechanisms of fuel cycle molecules like tetraoctyldiglycolamide (TODGA). Methods (120 words): The gas-phase fragmentation of protonated TODGA was investigated using collision-induced dissociation (CID), resonance ejection, and infrared ion spectroscopy (IRIS). CID and resonance ejection experiments were conducted using a Bruker Daltonics (Bremen, Gemany) SolariX XR fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer. IRIS spectra of protonated TODGA and its two CID fragmentation products were measured using a modified Bruker amaZon Speed ETD 3D quadrupole ion trap mass spectrometer coupled to the Free Electron Lasers for Infrared eXperiments (FELIX) free electron laser. Measured spectra were compared with density functional theory (DFT) calculations using the Gaussian 16, Revision C.02 software package with the ?B97X-D functional and def2-TZVPP basis sets. Candidate structures were generated using the CREST 3.0 conformational sampling software tool. Preliminary Data (300 words): Collision-induced dissociation of protonated TODGA ([C36H73N2O3]+, m/z=581.562) results two fragment ions, one at m/z=340.285 assigned as [C20H38NO3]+ and the other at m/z=312.290, assigned as [C19H38NO2]+. Based on the assigned formula and the structure of protonated TODGA, the fragment at m/z=340.285 is likely formed from elimination of neutral dioctylamine. Comparison of the IRIS spectrum of m/z=340.285 with DFT predictions suggests it contains a ring structure, and is assigned as N-octyl-N-(6-oxo-1,4-dioxan-2-ylidene)octan-1-aminium. Based on this structure and the structure of protonated TODGA, we hypothesize this fragment formed from elimination of neutral dioctylamine followed by a ring closure mechanism. Comparison of the IRIS spectrum of the fragment at m/z=312.290 with DFT predictions also indicated the presence of a ring structure, assigned as N-(1,3-dioxolan-4-ylidene)-N-octyloctan-1-aminium. This product could be formed from elimination of carbon monoxide from the ring of m/z=340.285 as a sequential fragmentation or formed directly from protonated TODGA via elimination of neutral N,N-dioctylformamide followed by a ring closure. Resonance ejection experiments where m/z=340 was continuously ejected from the IRC cell showed no decrease in intensity of m/z=312.290 across several collision energies, suggesting that the later, direct formation mechanism, dominates. The location of the ionizing proton in protonated TODGA is important for modeling the fragmentation mechanisms. DFT calculations suggested that the position of bands involving the coupled vibrations of the amide C—N and C=O bonds in TODGA are the most sensitive to proton location. Evaluation of the IRIS spectrum of protonated TODGA suggests that the ionizing proton is located between the two amid oxygens. This protonation location was calculated to lie approximately 30 kJ/mol lower in energy than the next lowest energy location, with the proton located solely on one of the amide oxygens. Novel aspect (20 words): Infrared ion spectroscopy combined with resonance ejection experiments and density functional theory to probe the collision-induced dissociation mechanism of tetraoctyldiglycolamide.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2024

Space radiation measurements during the Artemis I lunar mission

Space radiation is a notable hazard for long-duration human spaceflight. Associated risks include cancer, cataracts, degenerative diseases and tissue reactions from large, acute exposures. Space radiation originates from diverse sources, including galactic cosmic rays, trapped-particle (Van Allen) belts5 and solar-particle events. Previous radiation data are from the International Space Station and the Space Shuttle in low-Earth orbit protected by heavy shielding and Earth’s magnetic field and lightly shielded interplanetary robotic probes such as Mars Science Laboratory and Lunar Reconnaissance Orbiter. Limited data from the Apollo missions and ground measurements with substantial caveats are also available. Here we report radiation measurements from the heavily shielded Orion spacecraft on the uncrewed Artemis I lunar mission. At differing shielding locations inside the vehicle, a fourfold difference in dose rates was observed during proton-belt passes that are similar to large, reference solar-particle events. Interplanetary cosmic-ray dose equivalent rates in Orion were as much as 60% lower than previous observations. Furthermore, a change in orientation of the spacecraft during the proton-belt transit resulted in a reduction of radiation dose rates of around 50%. These measurements validate the Orion for future crewed exploration and inform future human spaceflight mission design.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1971

Observations of low-energy /0.3- to 1.8-MeV/ differential spectrums of trapped protons.

Measurements of differential energy spectrums of trapped protons obtained from several passes during the period January to November 1969 using the polar orbiting, low-altitude Injun 5 satellite equipped with a special solid-state detector proton-electron telescope are presented. Results reveal the existence of a quasi-persistent peak in the differential energy spectrum in the McIlwain shell parameter (L) range 2 to 2.6 and in the energy range of approximately 0.32 to 0.72 MeV. The fact that the shape of the spectrum is stable for several days or can change with time scales as small as 4 hours suggests an impulsive acceleration mechanism deep in the radiation belts. Other features of the spectrum show that if the spectrum is represented by an exponential form in energy, the dependence of the spectral parameter is in general agreement with diffusion theory over the L range of approximately 2 to 4.

Venkatesan, D.↗
NASA NTRS1993

Absorbed dose measurements and predictions on LDEF

The overall radiation environment of the Long Duration Exposure Facility (LDEF) was determined in part through the use of thermoluminescent detectors (TLD's) which were included in several experiments. The results given are from four experiments (A0015 Biostack, M0004 Fiber Optics Data Link, P0004 Seeds in Space, and P0006 Linear Energy Transfer Spectrum Measurement) and represent a large fraction of existing absorbed dose data. The TLD's were located on the leading and the trailing edges and the Earth end of the spacecraft under various shielding depths (0.48 to 15.4 g/sq cm). The measured absorbed doses were found to reflect both directional dependence of incident trapped protons and shielding. At the leading edge, doses ranged from 2.10 to 2.58 Gy under shielding of 2.90 to 1.37 g/sq cm Al equivalent (M0004). At the trailing edge, doses varied from 3.04 to 4.49 Gy under shielding of 11.7 to 3.85 g/sq cm (A0015), doses varied from 2.91 to 6.64 Gy under shielding of 11.1 to 0.48 g/sq cm (P0004), and a dose range of 2.66 to 6.48 Gy was measured under shielding of 15.4 to 0.48 g/sq cm (P0006). At the Earth end of the spacecraft, doses from 2.41 to 3.93 Gy were found under shielding of 10.0 to 1.66 g/sq cm (A0015). The effect of the trapped proton anisotropy was such that the western side of LDEF received more than 2 times the dose of the eastern side at shielding depths of approximately 1 g/sq cm. Calculations utilizing a directional model of trapped proton spectra predict smaller doses than those measured, being about 50 percent of measured values at the trailing edge and Earth end, and about 80 percent near the leading edge.

Frank, A. L.↗
DOE OSTI2022

Localized Excitation of Electromagnetic Ion Cyclotron Waves From Anisotropic Protons Filtered by Magnetic Dips

The excitation of electrostatic and/or electromagnetic waves in the plasma universe is often associated with anisotropic velocity distributions of charged particles. In Earth's inner magnetosphere, this anisotropy can gradually develop as particles injected from the magnetotail drift around the Earth at different speeds depending on their energy and pitch angle. Here, we show that the perpendicular-moving and bouncing ions can be separated more abruptly near the injection front. These pitch-angle filters are localized magnetic dip structures formed by the diamagnetic behavior of the injected particles, which can trap perpendicular-moving ions and allow bouncing ions to overtake. The resulting ion anisotropy facilitates the rapid generation of electromagnetic ion cyclotron (EMIC) waves, which in turn can largely reshape the Van Allen radiation belts. This scenario is examined by case and statistical observations, together with numerical simulations that reproduce most of the observational signatures, to support the causal relationship between magnetic dips, anisotropic ion distributions, and localized excitation of EMIC waves. Finally, our study highlights the important roles of magnetic dips in the inner magnetospheric dynamics, as pitch-angle filters of the injected ions and traveling hotspots of EMIC wave activities.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Effects of Proton Irradiation on the Performance of Skipper CCDs

Skipper CCDs are a mature detector technology that has been suggested for future space telescope instruments requiring sub-electron readout noise in the near-ultraviolet to the near-infrared. While modern skipper CCDs inherit from the radiation-tolerant p-channel detectors developed by LBNL, the effects of high doses of ionizing radiation on skipper CCDs (such as those expected in space) remains largely unmeasured. We report preliminary results on the performance of p-channel skipper CCDs following irradiation with 217-MeV protons at the Northwestern Medicine Proton Center. The total nonionizing energy loss (NIEL) experienced by the detectors exceeds 6 years at the Sun-Earth Lagrange Point 2 (L2). We demonstrate that the skipper amplifier continues to function as expected following this irradiation. Owing to the low readout noise of these detectors, controlled irradiation tests can be used to sensitively characterize the charge transfer inefficiency, dark current, and the density and time constants of charge traps as a function of proton fluence. We conclude with a brief outlook toward future tests of these detectors at other proton and gamma-ray facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

High-precision mass measurements of the isomeric and ground states of 44 V: Improving constraints on the isobaric multiplet mass equation parameters of the A=44, 0 + quintet

Background: The quadratic isobaric multiplet mass equation (IMME) has been very successful at predicting the masses of isobaric analog states in the same multiplet, while its coefficients are known to follow specific trends as functions of mass number. The Atomic Mass Evaluation 2016 [Chin. Phys. C 41, 030003 (2017)] 44 V mass value results in an anomalous negative c coefficient for the IMME quadratic term; a consequence of large uncertainty and an unresolved isomeric state. The b and c coefficients can provide useful constraints for construction of the isospin-nonconserving Hamiltonians for the pf shell. In addition, the excitation energy of the 0 + , T = 2 level in 44 V is currently unknown. This state can be used to constrain the mass of the more exotic 44 Cr. Purpose: The aim of the experimental campaign was to perform high-precision mass measurements to resolve the difference between 44 V isomeric and ground states, to test the IMME using the new ground state mass value and to provide necessary ingredients for the future identification of the 0 + , T = 2 state in 44 V. Method: High-precision Penning trap mass spectrometry was performed at LEBIT, located at the National Superconducting Cyclotron Laboratory, to measure the cyclotron frequency ratios of [ 44g,m VO] + versus [ 32 SCO] + , a well-known reference mass, to extract both the isomeric and ground state masses of 44 V. Results: The mass excess of the ground and isomeric states in 44 V were measured to be -23 804.9(80) keV/c 2 and -23 537.0(55) keV/c 2 , respectively. This yielded a new proton separation energy of S p = 1 773(10) keV. Conclusion: The new values of the ground state and isomeric state masses of 44 V have been used to deduce the IMME b and c coefficients of the lowest 2 + and 6 + triplets in A = 44. The 2 + c coefficient is now verified with the IMME trend for lowest multiplets and is in good agreement with the shell-model predictions using charge-dependent Hamiltonians. The mirror energy differences were determined between 44 V and 44 Sc, in line with isospin-symmetry for this multiplet. Finally, the new value of the proton separation energy determined, to an uncertainty of 10 keV, will be important for the determination of the 0 + , T = 2 state in 44 V and, consequently, for prediction of the mass excess of 44 Cr.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1991

Radiation exposure and dose estimates for a nuclear-powered manned Mars sprint mission

A conceptual manned mission to Mars is analyzed in order to estimate potential ionizing radiation doses that may be incurred by crew members during the course of the mission. The scenario is set for a journey during the solar active period and includes a brief stay on the Martian surface. Propulsion is assumed to be provided by nuclear thermal rocket power, and estimates of the dose contributions from the reactors are included. However, due to effective shielding of the reactors by large propellant tanks, it is found that the incurred doses are principally due to the charged particle natural environment. Recent data (August-December 1989) for large solar proton events are used to simulate the flame environment, while standard models are used for the trapped particle and galactic cosmic ray contributions. Shield effectiveness for several candidate materials are investigated.

Nealy, John E.↗
NASA NTRS1983

Ionic composition of the earth's radiation belts

Several different ion species have been positively identified in the earth's radiation belts. Besides protons, there are substantial fluxes of helium, carbon and oxygen ions, and there are measurable quantities of even heavier ions. European, American and Soviet space experimenters have reported ion composition measurements over wide ranges of energies: at tens of keV (ring-current energies) and below, and at hundreds of keV and above. There is still a gap in the energy coverage from several tens to several hundreds of keV where little observational data are available. In this review emphasis is placed on the radiation belt ionic structure above 100 keV. Both quiet time conditions and geomagnetic storm periods are considered, and comparison of the available space observations is made with theoretical analysis of geomagnetically trapped ion spatial, energy and charge state distributions.

Spjeldvik, W. N.↗
NASA NTRS2016

Radiation Tolerance Studies of Long Wavelength Infrared InAs/GaSb Detectors

In this work we investigated the effect of proton irradiation on the performance of long wavelength infrared (LWIR) InAs/GaSb photodiodes (λ(sub c) = 10.2µm) based on the complementary barrier infrared detector (CBIRD) design. We found that irradiation with 68MeV protons up to the total ionizing dose TID = 200 kRad results in only small (about 15%) decrease of the Quantum Efficiency and does not increase the operational bias of the photodiodes. However, the irradiation causes a significant increase of the dark current from j(sub d) = 5x10(exp -5) A/sq cm at V(sub b) = 0.1V and T = 80K to j(sub d) = 6x10(exp -3) A/sq cm at TID = 200 kRad. This change in the dark current mechanism can be attributed to the onset of surface leakage current, generated by the trap assisted tunneling processes in the proton displacement damage areas near the device sidewalls.

InAs/GaSb photodiodes↗
NASA NTRS2004

Survey of current situation in radiation belt modeling

The study of Earth's radiation belts is one of the oldest subjects in space physics. Despite the tremendous progress made in the last four decades, we still lack a complete understanding of the radiation belts in terms of their configurations, dynamics, and detailed physical accounts of their sources and sinks. The static nature of early empirical trapped radiation models, for examples, the NASA AP-8 and AE-8 models, renders those models inappropriate for predicting short-term radiation belt behaviors associated with geomagnetic storms and substorms. Due to incomplete data coverage, these models are also inaccurate at low altitudes (e.g., <1000 km) where many robotic and human space flights occur. The availability of radiation data from modern space missions and advancement in physical modeling and data management techniques have now allowed the development of new empirical and physical radiation belt models. In this paper, we will review the status of modern radiation belt modeling. Published by Elsevier Ltd on behalf of COSPAR.

Protons↗
NASA NTRS1972

Energetic protons in Jupiter's radiation belts

Estimates of the location, density, and energy of energetic protons in the Jupiter radiation belts are presented. A model of the Jupiter magnetosphere is developed by scaling from the Earth magnetosphere. Solar wind parameters, and magnetic and electric field characteristics in the magnetosphere are given for the Earth and projected for Jupiter. The upper limit of the number density of energetic protons is calculated to be 310,000/cu m, and the energy density would be about 310,000 MeV/cu m, or 51 nJ/cu m. A magnetic moment of 100 MeV/gauss for solar wind particles, a magnetic field on Jupiter's surface of 10 gauss, and a McIlwain parameter L of 7 are used. Sources of energetic particles are cosmic rays, satellite-magnetosphere interaction, and the solar wind, and their contributions are discussed. The two components of trapped energetic particle drift, one due to corotational and convective fields and the other due to gradients in the magnetic field, are described, and their periods are given.

Brice, N.↗
NASA NTRS1972

Diffusion models for Jupiter's radiation belt

Solutions are given for the diffusion of trapped particles in a planetary magnetic field in which the first and second adiabatic invariants are preserved but the third is not, using as boundary conditions a fixed density at the outer boundary (the magnetopause) and a zero density at an inner boundary (the planetary surface). Losses to an orbiting natural satellite are included and an approximate evaluation is made of the effects of the synchrotron radiation on the energy of relativistic electrons. Choosing parameters appropriate to Jupiter, the electrons required to produce the observed synchrotron radiation are explained. If a speculative mechanism in which the diffusion is driven by ionospheric wind is the true explanation of the electrons producing the synchrotron emission it can be concluded that Jupiter's inner magnetosphere is occupied by an energetic proton flux that would be a serious hazard to spacecraft.

Jacques, S. A.↗
NASA NTRS1974

Electrons and protons accelerated in Mercury's magnetic field

Fluxes of protons with energies of about 550 kev and electrons with energies of about 300 kev which exceed approximately 10,000 and 100,000 per sq cm per sec, respectively, have been discovered in the magnetosphere of Mercury. Electron fluxes greater than 1000 per sq cm per sec are also observed in the outbound pass of the Mariner 10 spacecraft through the magnetosheath. The intensity vs time profiles of the particle fluxes in the magnetosphere appear with sudden onsets beginning at interplanetary background levels and persisting for times equivalent to their being distributed spatially over regions having a scale size comparable to the planetary radius. It is shown that the radiation events observed in the magnetosphere and magnetosheath are transient and are not interpretable in terms of stable trapped particle populations.

Simpson, J. A.↗
NASA NTRS1995

A study of the radiation environment on board the space shuttle flight STS-57

A joint NASA-Russian study of the radiation environment inside a SPACEHAB 2 locker on space shuttle flight STS-57 was conducted. The shuttle flew in a nearly circular orbit of 28.5 deg inclination and 462 km altitude. The locker carried a charged particle spectrometer, a tissue equivalent proportional counter (TEPC), and two area passive detectors consisting of combined NASA plastic nuclear track detectors (PNTD's) and thermoluminescent detectors (TLD's), and Russian nuclear emulsions, PNTD's, and TLD's. All the detector systems were shielded by the same shuttle mass distribution. This makes possible a direct comparison of the various dose measurement techniques. In addition, measurements of the neutron energy spectrum were made using the proton recoil technique. The results show good agreement between the integral LET spectrum of the combined galactic and trapped particles using the tissue equivalent proportional counter and track detectors between about 15 keV/micron and 200 keV/micron. The LET spectrum determined from nuclear emulsions was systematically lower by about 50%, possibly due to emulsion fading. The results show that the TEPC measured an absorbed dose 20% higher than TLD's, due primarily to an increased TEPC response to neutrons and a low sensitivity of TLD's to high LET particles under normal processing techniques. There is a significant flux of high energy neutrons that is currently not taken into consideration in dose equivalent calculations. The results of the analysis of the spectrometer data will be reported separately.

Badhwar, G. D.↗
NASA NTRS1978

High-energy proton radiation damage of high-purity germanium detectors

Quantitative studies of radiation damage in high-purity germanium gamma-ray detectors due to high-energy charged particles have been carried out; two 1.0 cm thick planar detectors were irradiated by 6 GeV/c protons. Under proton bombardment, degradation in the energy resolution was found to begin below 7 x 10 to the 7th protons/sq cm and increased proportionately in both detectors until the experiment was terminated at a total flux of 5.7 x 10 to the 8th protons/sq cm, equivalent to about a six year exposure to cosmic-ray protons in space. At the end of the irradiation, the FWHM resolution measured at 1332 keV stood at 8.5 and 13.6 keV, with both detectors of only marginal utility as a spectrometer due to the severe tailing caused by charge trapping. Annealing these detectors after proton damage was found to be much easier than after neutron damage.

Pehl, R. H.↗
DOE OSTI2026

X-ray characterization of fully-depleted p-channel Skipper-CCDs for the DarkNESS mission

The Dark matter Nanosatellite Equipped with Skipper Sensors (DarkNESS) mission is a 6U CubeSat designed to search for X-ray lines from decaying dark matter using Skipper-CCDs. Thick, fully-depleted p-channel Skipper-CCDs provide low readout noise and high quantum efficiency for 1-10 keV X-rays, but their X-ray performance has not yet been demonstrated in the space environment. DarkNESS will operate in low-Earth orbit, where trapped protons induce displacement damage in the sensor that increases charge-transfer inefficiency and degrades the X-ray energy resolution. This work measures the X-ray line response of Skipper-CCDs before and after proton irradiation and quantifies the associated degradation. A sensor was exposed to 217 MeV protons at a fluence of 8.4 x 10^10 protons cm^-2, corresponding to a displacement-damage dose more than an order of magnitude above the three-year expectation for representative mid-inclination and Sun-synchronous low-Earth orbits. A 55Fe source was used to compare the energy resolution of the beam-exposed quadrant to adjacent unexposed quadrants and a non-irradiated reference sensor. These measurements provide a quantitative assessment of radiation-induced spectral degradation in Skipper-CCDs and enable an estimate of the end-of-life X-ray energy resolution expected for DarkNESS operation in low-Earth orbit.

Alpine, Phoenix [Illinois U., Urbana] (ORCID:00090↗
DOE OSTI2020

The “Hole” Story in Ionized Water from the Perspective of Ehrenfest Dynamics

The radiolysis of liquid water and the radiation-matter interactions that happen in aqueous environments are important to the elds of chemistry, materials, and environmental sciences, as well as biological and physiological response to extreme conditions and medical treatments. The initial stage of radiolysis is the ultrafast response, or hole dynamics, that trigger chemical processes within complex energetic landscapes that may include reactivity. A fundamental understanding necessitates the use of theoretical methods that are capable of simulating both ultrafast coherence and non-adiabatic energy transfer pathways. In this work, we carry out an ab initio Ehrenfest dynamic study in order to provide a more complete description of the ultrafast dynamics and reactive events initiated by photoionization of water. Furthermore, after sudden ionization, the range of processes that include hole trapping and transfer, large OH oscillations, proton transfer and subsequent relay, formation of the metastable Zundel complex, and long-lived coherence, are identied and new insight into their driving forces are elucidated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗