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All sourcesNASA NTRSDOE OSTI
NASA NTRS1998

Chemical composition measurements of the atmosphere of Jupiter with the Galileo Probe mass spectrometer

The Galileo Probe entered the atmosphere of Jupiter on December 7, 1995. Measurements of the chemical and isotopic composition of the Jovian atmosphere were obtained by the mass spectrometer during the descent over the 0.5 to 21 bar pressure region over a time period of approximately 1 hour. The sampling was either of atmospheric gases directly introduced into the ion source of the mass spectrometer through capillary leaks or of gas, which had been chemically processed to enhance the sensitivity of the measurement to trace species or noble gases. The analysis of this data set continues to be refined based on supporting laboratory studies on an engineering unit. The mixing ratios of the major constituents of the atmosphere hydrogen and helium have been determined as well as mixing ratios or upper limits for several less abundant species including: methane, water, ammonia, ethane, ethylene, propane, hydrogen sulfide, neon, argon, krypton, and xenon. Analysis also suggests the presence of trace levels of other 3 and 4 carbon hydrocarbons, or carbon and nitrogen containing species, phosphine, hydrogen chloride, and of benzene. The data set also allows upper limits to be set for many species of interest which were not detected. Isotope ratios were measured for 3He/4He, D/H, 13C/12C, 20Ne/22Ne, 38Ar/36Ar and for isotopes of both Kr and Xe.

unmanned↗
NASA NTRS1992

How Mars lost its atmosphere

There is a widespread suspicion that Mars thin atmosphere is in some way attributable to the planet's size. Another possibility is that the atmosphere was never degassed or outgassed in the first place. I prefer escape. Hydrodynamic escape (vigorous thermal escape) and impact erosion (expulsion of atmosphere by impacts) are two processes that should have been operative early. Although in principle hydrodynamic escape could have shrunk Mars atmosphere a hundredfold while leaving the composition of the remnant atmosphere nearly unaltered, very high escape fluxes are required. The implicated escape mechanism must have been efficient, nearly non-fractionating, and vastly more potent for Mars than for Earth or Venus. Impact erosion is an appealing candidate. Noble gases are the obvious first test. Noble gases are the most volatile elements and so are the most likely to have been affected by impact erosion and the easiest to address quantitatively. Xenon in particular imposes three constraints on how Mars lost its atmosphere: (1) the very low abundance of nonradiogenic Xe abundance of nonradiogenic Xe compared to Earth, Venus, and likely meteoritic sources; (2) its nonradiogenic isotopes distinct from likely meteoritic sources; and (3) the relatively high absolute abundance of radiogenic daughter of the extinct radionuclide I-129 (half-life 17 Myr). In impact erosion, the first two become constraints on the composition, mass distribution, and orbital elements of the impactors. The third requires that Mars lost its nonradiogenic Xe early, probably before it was 100 Myr old. Impact erosion can explain Mars by any of three stories. (1) Mars in unlikely. In a sort of planetary brinkmanship, impact erosion almost removed the entire atmosphere but was arrested just in time. (2) Martian noble gases are cometary and cometary Xe is as isotopically mass fractionated as Martian and terrestrial Xe. This is most easily accomplished if a relatively thick geochemically controlled CO2 atmosphere protected trace atmophiles against escape. (3) Mars was indeed stripped of its early atmosphere but a small remnant was safely stored in the regolith, later released as a byproduct of water mobilization.

Zahnle, Kevin↗
NASA NTRS1981

Nitrogen isotopes in the Allende meteorite

Nitrogen in the Allende meteorite consists of at least two components, partially resolvable in a stepwise heating experiment. L-nitrogen, released below 1000 C, has a low delta N-15 (-60 to -90 per mil), and is associated with neon-A and CCF-xenon and may reside in a carbonaceous carrier. H-nitrogen, released above 1000 C, is associated with normal xenon, and may reside in silicate minerals. It is very difficult to account for the entire range of N-15/N-14 ratios in solar system materials by mass-dependent chemical and physical processes alone. In particular, an N-14 enriched component of nuclear origin appears necessary to account for the L-nitrogen in Allende.

Thiemens, M. H.↗
DOE OSTI2022

A dry ancient plume mantle from noble gas isotopes

Primordial volatiles were delivered to terrestrial reservoirs during Earth’s accretion, and the mantle plume source is thought to have retained a greater proportion of primordial volatiles compared with the upper mantle. This study shows that mantle He, Ne, and Xe isotopes require that the plume mantle had low concentrations of volatiles like Xe and H 2 O at the end of accretion compared with the upper mantle. A lower extent of mantle processing alone is not sufficient to explain plume noble gas signatures. Ratios of primordial isotopes are used to determine proportions of solar, chondritic, and regassed atmospheric volatiles in the plume mantle and upper mantle. The regassed Ne flux exceeds the regassed Xe flux but has a small impact on the mantle Ne budget. Pairing primordial isotopes with radiogenic systems gives an absolute concentration of 130 Xe in the plume source of ∼1.5 × 10 7 atoms 130 Xe/g at the end of accretion, ∼4 times less than that determined for the ancient upper mantle. A record of limited accretion of volatile-rich solids thus survives in the He-Ne-Xe signatures of mantle rocks today. A primordial viscosity contrast originating from a factor of ∼4 to ∼250 times lower H 2 O concentration in the plume mantle compared with the upper mantle may explain (a) why giant impacts that triggered whole mantle magma oceans did not homogenize the growing planet, (b) why the plume mantle has experienced less processing by partial melting over Earth’s history, and (c) how early-formed isotopic heterogeneities may have survived ∼4.5 Gy of solid-state mantle convection.

58 GEOSCIENCES↗
NASA NTRS1974

Clues in the rare gas isotopes to early solar system history

Rare gases in meteorites and lunar samples are discussed stimulating the discovery of the solar wind. Radioactive isotopes are examined, making a correlation to the origin of the solar system. It is shown that the heights of the peaks above the horizontal lines represent the spectrum of the fissiogenic sample. Nuclear tracks of iodine, xenon, and plutonium detected in lunar rocks are also explained.

Reynolds, J. H.↗
DOE OSTI2020

Modeling of fission and activation products in molten salt reactors and their potential impact on the radionuclide monitoring stations of the International Monitoring System

Molten Salt Reactors (MSRs) are one of six Generation IV reactor designs currently under development around the world. Because of the unique operating conditions of MSRs, which include molten fuel and the continuous removal of gaseous fission products during operation, work was performed to analyze the potential impact of emissions on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Simulations were performed to predict the production of IMS-relevant radionuclides in four MSR designs operating under two scenarios – (1) a sealed reactor with releases only during operational shutdown and (2) continuous reprocessing or sparging of the fuel salt. From these production estimates the radioxenon and radioiodine signatures were extracted and compared to three current reactor designs (PWR, BWR, RBMK). In the cases where continuous reprocessing of the fuel salt occurred both the radioxenon and radioiodine signatures are nearly indistinguishable from a nuclear explosion. Estimates were also made of the potential emission rate of radioxenon for three reactor designs and it was found that MSRs have the potential to emit radioxenon isotopes at a rate of 1015 – 8×1016 Bq/d for 133Xe if no abatement is used. An assessment was also made of activation products using a candidate fuel salt (FLiBe) mixed with corrosion products for the Thorium Molten Salt Reactor (TMSR-LF1)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
NASA NTRS1973

Extinct lunar radio activities - Xenon from Pu-244 and I-129 in Apollo 14 breccias.

Two Apollo 14 breccias have been found to contain xenon from the spontaneous fission of 82 my Pu-244. A third contains 60 times as much fission xenon as local uranium can account for and is probably of similar character. One of the breccias shows a Xe-129 excess most likely due to the decay of 17 my I-129. That these components can be separated and identified at all implies that complete isotopic homogenization has not occurred over a period which encompasses both extinction of these radionuclides and compaction of the breccias into their final form. In this sense isotope pre-history has been preserved in some lunar breccias providing information that pre-dates the formation of the rock itself (as determined by conventional techniques).

Behrmann, C. J.↗
DOE OSTI2021

Examining Nuisance Aerosol Detections in Light of the Origin of the Screening Process (November 2021)

The evolution of philosophy and computations in the International Data Center (IDC) related to aerosol samples have had profound impacts on the number of recorded detections in the network since routine operations began in 2000. Key decisions from policymakers have been the list of triggering radionuclides, the scheme for categorizing these into interest levels 1-5, and an algorithm for determining when an anthropogenic isotope is seen so often that it is no longer interesting, known as the Exponential Weighted Moving Average (EWMA). These are described in the Operations Manual of the IDC. Key parameters that are controlled by the IDC but for which the IDC receives occasional input from policymakers include the constants in EWMA and the peak significance threshold for individual gamma rays, the latter of which directly leads to determination of the presence or absence of a radionuclide in a sample. There are also changes in computations which the IDC makes and informs policy makers about, such as changes in how background is computed, which could also affect the ease of detecting a peak – real or false. Rather than focus on the quantitative changes due to computation changes, this work records some thinking on how isotopes and peak significance levels were chosen, and the resulting detections seen over 18 years during the buildup of the International Monitoring System (IMS). These detections are considered on a global scale to try to determine the relative impact on monitoring, and in some cases, the nature of their existence. Repeated detections of 131I and 133I are the most troublesome, but they are not so frequent to be a major problem for the Verification Regime. These detections could probably be handled adequately using scientific methods currently under development for xenon backgrounds. It is also somewhat problematic that top-level analysis of aerosol backgrounds has not been reported previous to this. The steep increase in the rate of detections after 2016 are a concern, either in the actual backgrounds or from changes in the calculations methods used to generate the Reviewed Radionuclide Report (RRR.) Final conclusions of the authors are that the computational stability of the RRR is very important. With computational stability, changes can be usefully analyzed as being due to changes in radioactivity in Earth’s atmosphere This report is a distillation into text of a talk given in the Radionuclide Experts Group (RNEG) in Vienna during Working Group B (WGB) in February of 2019. This report does not directly contain any IDC data, only summaries by year, or by isotope, or by location. No specific IDC detection by time, location, or isotope is included.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Photonuclear Production of Radioxenon for Air Samples

Radioxenon plays an important role in ensuring compliance with the Comprehensive Nuclear-Test-Ban Treaty due to its ability to be transported through the atmosphere, as well as the fact that the half-lives of its isotopes provide a window long enough to be detected but not long enough that it could become background radiation. This allows it to be correlated with specific events that indicate the testing of nuclear weapons. Idaho National Laboratory supports this mission by providing spiked air samples for monitoring stations to enable instrument calibration and ensure measurement accuracy. We tested a photonuclear method of producing one of the main isotopes of radioxenon, Xe-135. We also tested the separation of Xe-135 from the parent isotope Xe-136 using the method of kinematic recoil. Aluminum coils were placed in quartz ampoules filled with enriched Xe-136 and were irradiated by a bremsstrahlung beam with an endpoint energy of 21 MeV. The results showed that we were not only successful in producing Xe-135 but also that the Xe-135 was deposited into the coil allowing it to be removed from the Xe-136 gas. The coil and the Xe-135 can then be chemically separated. At the time of counting the coil, it was calculated that there was about 18 Bq of activity from Xe-135 remaining in the coil. Future work includes determining the optimal material and geometry of the catcher to maximize the amount of Xe-135 captured.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

First Simultaneous Acceleration of Multiple Charge States of Heavy Ion Beams in a Large-Scale Superconducting Linear Accelerator

Experimental studies of the simultaneous acceleration of three-charge-state 129 Xe 49+,50+,51+ beam from 17 to 180 MeV/nucleon in a superconducting linear accelerator are presented. The beam parameters for each individual- and multiple-charge-state beam were measured and compared with the particle tracking simulations. Detailed measurements were performed to characterize the multiple-charge-state beam’s recombination after a second-order achromat and isopath 180° bending system. As a result of the recombination of three charge states in the six-dimensional phase space, the xenon beam intensity was increased by 2.5-fold compared to the single-charge-state beam. Lastly, the results presented in the Letter fully validate the possibility to produce and utilize high-quality multiple-charge-state heavy-ion beams in a large-scale superconducting linac to increase the available beam power on an isotope production target.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Aggregation of solutes in bosonic versus fermionic quantum fluids

Quantum fluid droplets made of helium-3 ( 3 He) or helium-4 ( 4 He) isotopes have long been considered as ideal cryogenic nanolabs, enabling unique ultracold chemistry and spectroscopy applications. The droplets were believed to provide a homogeneous environment in which dopant atoms and molecules could move and react almost as in free space but at temperatures close to absolute zero. Here, we report ultrafast x-ray diffraction experiments on xenon-doped 3 He and 4 He nanodroplets, demonstrating that the unavoidable rotational excitation of isolated droplets leads to highly anisotropic and inhomogeneous interactions between the host matrix and enclosed dopants. Superfluid 4 He droplets are laced with quantum vortices that trap the embedded particles, leading to the formation of filament-shaped clusters. In comparison, dopants in 3 He droplets gather in diffuse, ring-shaped structures along the equator. The shapes of droplets carrying filaments or rings are direct evidence that rotational excitation is the root cause for the inhomogeneous dopant distributions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1977

Planetary noble gas components in Orgueil

In the reported investigation, the approach employed by Jeffery and Anders (1970) and Eberhardt (1974), who used colloidal suspensions in separating minerals of the Orgueil carbonaceous chondrite (C1), was extended to an application involving the enrichment of a planetary noble gas carrier in several C1 and C2 meteorites. The thermal release pattern of Orgueil 'carbon' is considered, taking into account elemental effects, a comparison of noble gas release from 'carbon' separates and bulk meteorite samples, isotopic effects, and a comparison with Murray 'carbon'. An evaluation is conducted of the noble gas components in carbonaceous chondrites. The origin of primordial noble gases in carbonaceous chondrites is also discussed, giving attention to the origin of solar gases, the role of 'carbon' as the novel vehicle for planetary gases, and plausible astrophysical sites for the production of anomalous krypton and xenon.

Frick, U.↗
DOE OSTI2024

133Xe Noble Gas Mass Spectrometry Measurement for High Purity Germanium Detector Performance Verification

Idaho National Laboratory produces quality control standards for laboratories that operate xenon radionuclide monitoring systems. Activities reported with each quality control standard are quantified using high purity germanium detectors. A collection of measurement capabilities are being set up at Idaho National Laboratory to establish an in-house high purity germanium detector performance verification system, with noble gas mass spectrometry being one of these measurement capabilities. The first noble gas mass spectrometry and high purity germanium measurement comparison is presented here. A Xe-133 gas sample was prepared and the activity was quantified with high purity germanium detectors. The Xe-133 sample was diluted with a known quantity of isotopically enriched Xe-126 gas; the resulting Xe-133 : Xe-126 atom ratio was calculated to be 1.15x10-4 +/- 2% at reference time t. An aliquot of this gas sample containing approximately 10 million Xe-133 atoms was introduced into a ThermoFisher Scientific Helix MC Plus noble gas mass spectrometer for analysis. The measured Xe-133 : Xe-126 atom ratio was determined to be 1.10x10-4 +/- 2% (1-sigma uncertainty) at reference time t, about 4.3% lower than the atom ratio determined with the measured high purity germanium activity.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
NASA NTRS1996

The Galileo probe mass spectrometer: composition of Jupiter's atmosphere

The composition of the jovian atmosphere from 0.5 to 21 bars along the descent trajectory was determined by a quadrupole mass spectrometer on the Galileo probe. The mixing ratio of He (helium) to H2 (hydrogen), 0.156, is close to the solar ratio. The abundances of methane, water, argon, neon, and hydrogen sulfide were measured; krypton and xenon were detected. As measured in the jovian atmosphere, the amount of carbon is 2.9 times the solar abundance relative to H2, the amount of sulfur is greater than the solar abundance, and the amount of oxygen is much less than the solar abundance. The neon abundance compared with that of hydrogen is about an order of magnitude less than the solar abundance. Isotopic ratios of carbon and the noble gases are consistent with solar values. The measured ratio of deuterium to hydrogen (D/H) of (5 +/- 2) x 10(-5) indicates that this ratio is greater in solar-system hydrogen than in local interstellar hydrogen, and the 3He/4He ratio of (1.1 +/- 0.2) x 10(-4) provides a new value for protosolar (solar nebula) helium isotopes. Together, the D/H and 3He/4He ratios are consistent with conversion in the sun of protosolar deuterium to present-day 3He.

NASA Discipline Number 52-10↗
DOE OSTI2025

Influence of background sources and topographic resolution in the Weather Research and Forecasting Model on xenon plume characteristics at monitoring stations

For many atmospheric monitoring applications, networks of measurement sites—such as the radionuclide stations of the International Monitoring System—can be sparse. With measurement locations potentially hundreds to thousands of kilometers from a release it is important to quantify the effects of physical processes on transport and dispersion of plumes between source and measurement locations. This study addresses the effects of background sources and topography resolution near the release location of radionuclides. We use the Weather Research and Forecasting (WRF) model with inline chemistry to investigate (1) how an additional, time-varying source of 133 Xe, such as an operational medical isotope production facility, contributes to activity concentration measurements at monitoring sites, and (2) how complex topography influences on atmospheric conditions near emission sources impact plume concentrations at varying distances from the source. Two 133 Xe emission sources, including (1) a high flux rate of short duration representing an explosive event, and (2) a variable and continuous background source, are simulated. The continuous background source contributes significantly to total 133 Xe concentrations at several monitoring stations. Further, a WRF simulation at 9 km horizontal resolution is compared with a nested grid simulation, where the innermost domain has a resolution of 1 km. Increased topographic resolution leads to an improved representation of plume responses to local winds, with topographic influences greatest at locations closest to the sources. Differences between the two domain resolutions decrease at greater distances from the sources, as plumes have time to spread and mix and are influenced by synoptic scale circulation patterns that are represented similarly in both simulations.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2010

The Composition of Titan's Lower Atmosphere and Simple Surface Volatiles as Measured by the Cassini-Huygens Probe Gas Chromatograph Mass Spectrometer Experiment

The Cassini-Huygens Probe Gas Chromatograph Mass Spectrometer (GCMS) determined the composition of the Titan atmosphere from ~140km altitude to the surface. After landing, it returned composition data of gases evaporated from the surface. Height profiles of molecular nitrogen (N2), methane (CH4) and molecular hydrogen (H2) were determined. Traces were detected on the surface of evaporating methane, ethane (C2H6), acetylene (C2H2), cyanogen (C2N2) and carbon dioxide (CO2). The methane data showed evidence that methane precipitation occurred recently. The methane mole fraction was (1.48+/-0.09) x 10(exp -2) in the lower stratosphere (139.8 km to 75.5 km) and (5.65+/-0.18) x 10(exp -2) near the surface (6.7 km to the surface). The molecular hydrogen mole fraction was (1.01+/-0.16) x 10(exp -3) in the atmosphere and (9.90+/-0.17) x 10(exp -4) on the surface. Isotope ratios were 167.7+/-0.6 for N-14/N-15 in molecular nitrogen, 91.1+/-1.4 for C-12/C-13 in methane and (1.35+/-0.30) x 10(exp -4) for D/H in molecular hydrogen. The mole fractions of Ar-36 and radiogenic Ar-40 are (2.1+/-0.8) x 10(exp -7) and (3.39 +/-0.12) x 10(exp -5) respectively. Ne-22 has been tentatively identified at a mole fraction of (2.8+/-2.1) x 10(exp -7) Krypton and xenon were below the detection threshold of 1 x 10(exp -8) mole fraction. Science data were not retrieved from the gas chromatograph subsystem as the abundance of the organic trace gases in the atmosphere and on the ground did not reach the detection threshold. Results previously published from the GCMS experiment are superseded by this publication.

Niemann, H. B.↗
NASA NTRS1979

Isotopic anomalies of noble gases in meteorites and their origins. III - LL-chondrites

Nine LL-chondrites were studied by selective etching to characterize the noble gas components in three mineral fractions: HF-HCl-solubles, chromite and carbon. The Ne-20/Ar-36 ratio is considered, noting that chondrites of different petrologic types cannot all be derived from the same volatile rich ancestor, but must have formed over a range of temperatures, with correspondingly different volatile contents. Variations in the carbonaceous chondrite fission (CCFXe) component in LL3, LL5, and LL6 chondrites are discussed, noting that if CCFXe comes from a supernova, then its distribution in LL-chondrites requires three presolar carrier minerals of the right solubility properties, containing three different xenon components. However, if CCFXe comes from fission of a volatile superheavy element, then its decrease from LL3 to LL6 can be attributed to less complete condensation from the solar nebula. Finally, the three types of primordial xenon components which occur in different minerals of the same meteorite are described.

Alaerts, L.↗
DOE OSTI2023

Noble gas constraints on spent fuel irradiation histories

Fission gas isotopic compositions are sensitive to a variety of reactor operating parameters that include the neutron flux, neutron fluence at different neutron energies, and operating temperature. Measurements of fission gas isotopic compositions thus have potential to constrain reactor simulations for nuclear forensics and safeguards applications. In this paper, we present Kr and Xe isotope measurements from a suite of samples obtained from locations that span the axial length a fuel pin with a well-characterized irradiation history and compare these data to spatially resolved reactor simulations. Here, we observed positive correlations between fluence sensitive isotopic ratios and burnup and between a flux sensitive ratio and power, although some discrepancies are observed between the measured data and model predictions. These differences may be due to simplifications in the model and/or inaccuracies in the cross sections. A much broader measurement to model comparison is required to better understand the discrepancies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗