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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗
DOE OSTI2026

A comparison of long-term 37 Ar and 39 Ar transport and implications for 39 Ar as a persistent indicator of underground nuclear explosions

Measurements were first made in 2016 of legacy 39 Ar gas from the decades-old Barnwell underground nuclear explosion site within the Nevada National Security Site. This has raised the question of the ubiquity of the radionuclide 39 Ar following underground nuclear explosions in general locations. This article presents a high-level evaluation of the scientific case for using 39 Ar as a long-term indicator of underground nuclear explosions. Assessment is made based on a broad set of assumptions to reasonably estimate the persistence of 39 Ar in the subsurface environment following an explosion to establish potential detectability years to decades after the originating event.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Evaluation of cosmogenic production of 39 Ar and 42 Ar for rare-event physics using underground argon

Underground argon (UAr) with lower cosmogenic activities of 39 Ar and 42 Ar has been planned as a detector in detecting scintillation light and charge collection using time projection chambers for dark matter searches and as a veto detector in suppressing backgrounds for neutrinoless double beta decay (0$vββ$ ) experiments. Long-lived radioactive isotopes, 39 Ar and 42 Ar, can also be produced on the surface when UAr is pumped out from a deep well. Understanding the production of long-lived isotopes in Ar is important for utilizing UAr for dark matter and 0$vββ$ experiments in terms of its production, transportation, and storage. Ar exposure to cosmic rays at sea-level is simulated using Geant4 for a given cosmic ray muon, neutron, and proton energy spectrum. Here we report the simulated cosmogenic production rates of 39 Ar, 42 Ar, and other long-lived isotopes at sea-level from fast neutrons, high energy muons, and high energy protons. Total production rates of 938.53/kg Ar day and 5.81 × 10 -3 /kg Ar day for 39 Ar and 42 Ar are found from our simulation. Utilizing these production rates, we set a time limit of 954 days constrained by the production of 39 Ar for UAr to be on the surface before it compromises the sensitivity for a dark matter experiment. Similarly, a time limit of 1702 days constrained by the production of 42 Ar is found for a 0$vββ$ experiment.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

The 40 Ar(d,p) 41 Ar cross section between 3–7 MeV

To determine the safety of using argon as a deuteron beam stopping material, the 40 Ar(d,p) 41 Ar cross section was measured at average deuteron energies of 3.6 MeV, 5.5 MeV, and 7.0 MeV using an activation method. A 16-MeV deuteron beam produced by Lawrence Berkeley National Laboratory’s 88-Inch Cyclotron was degraded to each energy by nickel foils and the front wall of an aluminum gas chamber. The reduced-energy deuterons were used to activate a sample of nat Ar gas. After each irradiation, the gas chamber’s 41 Ar activation was measured with a high-purity germanium detector. The cross sections measured were larger than a previous measurement by ~40%.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Separating $${^{39}\hbox {Ar}}$$ from $${^{40}\hbox {Ar}}$$ by cryogenic distillation with Aria for dark-matter searches

Abstract Aria is a plant hosting a $${350}\,\hbox {m}$$ 350 m cryogenic isotopic distillation column, the tallest ever built, which is being installed in a mine shaft at Carbosulcis S.p.A., Nuraxi-Figus (SU), Italy. Aria is one of the pillars of the argon dark-matter search experimental program, lead by the Global Argon Dark Matter Collaboration. It was designed to reduce the isotopic abundance of $${^{39}\hbox {Ar}}$$ 39 Ar in argon extracted from underground sources, called Underground Argon (UAr), which is used for dark-matter searches. Indeed, $${^{39}\hbox {Ar}}$$ 39 Ar is a $$\beta $$ β -emitter of cosmogenic origin, whose activity poses background and pile-up concerns in the detectors. In this paper, we discuss the requirements, design, construction, tests, and projected performance of the plant for the isotopic cryogenic distillation of argon. We also present the successful results of the isotopic cryogenic distillation of nitrogen with a prototype plant.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

First Measurement of $π^+$-Ar and $p$-Ar Total Inelastic Cross Sections in the Sub-GeV Energy Regime with ProtoDUNE-SP Data

The ProtoDUNE-SP detector, a kiloton-scale prototype for the Deep Underground Neutrino Experiment (DUNE), is the largest liquid argon time projection chamber built to date. Operated at CERN from 2018 to 2020, it collected both cosmic-ray data and a beam consisting of positively-charged particles with discrete momentum settings across a range of 0.3 GeV/$c$ to 7 GeV/$c$. In this letter, we report the total inelastic cross section measurements for $π^+$-Ar and $p$-Ar interactions using selected $π^+$ and proton samples from the 1 GeV/$c$ beam data. These results provide the first measurement of the total inelastic cross sections for $π^+$-Ar in the 500-900 MeV kinetic energy range and for $p$-Ar below 450 MeV, both of which are directly relevant to the DUNE energy range. The measured cross sections are consistent with predictions and provide a dataset that was previously unavailable for argon targets. These measurements are essential for constraining neutrino-argon interaction models, which are crucial for the precision physics goals of the upcoming DUNE experiment.

Abbaslu, Saeed [IPM, Tehran] (ORCID:00000003356771↗
DOE OSTI2021

Analysis of the Ion Conversion Mechanisms in the Effluent of Atmospheric Pressure Plasma Jets in Ar with Admixtures of O 2 , H 2 O and Air

Ionic species in atmospheric pressure plasma jets (APPJs) play an important role in plasmasurface and plasma-liquid interactions, nonetheless, they have not received the same attention as their neutral reactive species counterparts. In this work, a molecular beam mass spectrometer (MBMS) was used to characterize the ion compositions in the effluent of an APPJ operating in ambient air for different feed gases including Ar + O 2 , Ar + air and Ar + H 2 O mixtures inspired by gas compositions used for biomedical applications. Changes in compositions of positive and negative ions as a function of nozzle-to-substrate distance along the plasma plume were analyzed and compared with a pseudo-1D plug flow model. Positive and negative ions were detected up to distances of 12 mm from the visible plasma plume tip. The measurements enable to follow the ion conversion pathways in the effluent of the APPJs as a function of distance from the nozzle. The trends in ion yield obtained from a pseudo-1D plug flow model showed generally a good agreement with the experimentally observed trends after addition of ionic reactions to the previously reported reaction set but also some distinctive differences were observed. The dominant positive ions in the far effluent are water ion clusters, the most stable ion for all gas mixtures investigated, while a large variety of negative ions was found for different gas mixtures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Detrital U-Pb zircon and 40 Ar/ 39 Ar muscovite geochronology from Middle Pennsylvanian strata in the Anadarko Basin, Texas Panhandle, USA

The Late Mississippian-Permian Anadarko Basin formed in Texas and Oklahoma, USA as the result of inversion of Neoproterozic and Cambrian rift structures. Subsidence was driven by flexural loading of the Amarillo-Wichita Uplift, and this uplift may represent the easternmost element of the Ancestral Rocky Mountains system. The northwestern part of this basin has generally been interpreted to have been filled by sediment derived from the Ancestral Front Range Uplift, ~475 km to the northwest during the early stages of basin filling. We test this model using U-Pb detrital zircon and 40 Ar/ 39 Ar detrital muscovite results from three subsurface samples of the Morrow B sandstone in the northwestern part of the Anadarko Basin. We provide a new maximum depositional age of 310.9 ± 4.9 Ma that indicates the age of the Morrow B to be no older than late Atokan to early Desmoinesian Age (Moscovian), ~10 Myr younger than previously interpreted. In contrast to some previous interpretations, we propose that the most likely source for the sediment in the Morrow B is the Amarillo Uplift to the south. Detrital zircon and detrital muscovite data have age peaks at 900–1300 Ma, 1370 Ma and 1600–1800 Ma corresponding to derivation from Grenville, Granite-Rhyolite and Yavapai-Mazatzal basement provinces, respectively. A dominant detrital zircon peak at 1370 Ma suggests that Mesoproterozoic granites in the Amarillo Uplift were exposed by Middle Pennsylvanian time, and detritus eroded from the Amarillo Uplift dominated the lowstand sediment budget of the Texas Panhandle during this time; small volumes of sediment were likely sourced from the Ancestral Front Range. In conclusion, this study presents the first detrital geochronology data from the subsurface Anadarko Basin and the first detrital muscovite data from late Paleozoic southwestern Laurentia. The results presented here highlight the interpretive power of combined detrital zircon and muscovite datasets.

58 GEOSCIENCES↗
DOE OSTI2026

Plasma decay of nanosecond pulsed laser-produced Ar and Ar–H 2 O sparks at atmospheric pressure

Time-resolved diagnostics were applied to investigate free-electron properties in nanosecond laser-produced discharges generated in atmospheric pressure Ar and in Ar–3%H 2 O. The discharges were generated using 23 ns, 1064 nm laser pulses. Broadband plasma imaging and laser Thomson scattering were combined with optical emission spectroscopy, with particular emphasis on the Stark broadening of the H α and H β lines. The plasma exhibited a bright emission that persists for up to 30–40 µs after breakdown. Plasma emission was then followed by a very weak glow emission that persisted for up to 19 ms after breakdown. Peak electron number density of ∼2 × 10 17 cm −3 and electron temperature of ∼7 eV were measured. An excellent agreement between both techniques was obtained regarding absolute electron number densities. The inferred free-electron temporal decay dynamics are consistent with processes dominated by hydrodynamic expansion and two- and three-body electron–ion recombination. These results provide benchmark data for modeling nanosecond laser discharges and demonstrate the reliability of combining Thomson scattering with Stark broadening in atmospheric laser sparks.

Thomson scattering↗
DOE OSTI2020

Interpreting and reporting 40 Ar/ 39 Ar geochronologic data

The 40Ar/39Ar dating method is among the most versatile of geochronometers, having the potential to date a broad variety of K-bearing materials spanning from the time of Earth’s formation into the historical realm. Measurements using modern noble-gas mass spectrometers are now producing 40Ar/39Ar dates with analytical uncertainties of ~1%, thereby providing precise time constraints for a wide range of geologic and extraterrestrial processes. Analyses of increasingly smaller subsamples have revealed age dispersion in many materials, including some minerals used as neutron fluence monitors. Accordingly, interpretive strategies are evolving to address observed dispersion in dates from a single sample. Moreover, inferring a geologically meaningful “age” from a measured “date” or set of dates is dependent on the geological problem being addressed and the salient assumptions associated with each set of data. We highlight requirements for collateral information that will better constrain the interpretation of 40Ar/39Ar data sets, including those associated with single-crystal fusion analyses, incremental heating experiments, and in situ analyses of microsampled domains. To ensure the utility and viability of published results, we emphasize previous recommendations for reporting 40Ar/39Ar data and the related essential metadata, with the amendment that data conform to evolving standards of being findable, accessible, interoperable, and reusable (FAIR) by both humans and computers. Our examples provide guidance for the presentation and interpretation of 40 Ar/ 39 Ar dates to maximize their interdisciplinary usage, reproducibility, and longevity.

58 GEOSCIENCES↗
DOE OSTI2021

Measurements of emanation of Ar-37 and Ar-39 from irradiated rocks and powders

The emanation fraction of radionuclides has been highlighted as a known source of uncertainty in the estimation of radionuclide source signatures from underground nuclear tests and other nuclear activities, particularly in the case of activation products. A system was developed at Pacific Northwest National Laboratory to quantify the emanation fraction of argon from samples ranging in particle size from powder to small rocks. Seven materials, two powders and five rock types, were irradiated with fission spectrum neutrons and the emanation fraction of 37 Ar was measured. Additional measurements were made of the 39 Ar emanation for four of these materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ion fluxes and memory effects in an Ar–O 2 modulated radiofrequency-driven atmospheric pressure plasma jet

In this work we used molecular beam mass spectrometry to characterize ion fluxes produced by a modulated radiofrequency (RF)-driven atmospheric pressure plasma jet operating in a homogeneous gas environment (Ar + 1% O 2 ). The influence of the RF modulation frequency (100 Hz to 20 kHz) on the ion fluxes was investigated by time-resolved measurements, and the lifetimes of the dominant ions, O 2 + , NO + , O − , O 2 − and O 3 − , were found to be 28 ± 2, 117 ± 8, 7.3 ± 0.4, 17 ± 1 and 23 ± 2 μs, respectively. The absolute ion densities in the near afterglow region were found to be of the order of 1011 cm−3. Significant differences in the dynamics of the positive and negative ions were found; these are explained by the presence of electrons at similar densities in the afterglow produced by electron detachment reactions from negative ions due to the large concentrations of atomic oxygen and singlet delta oxygen. Transitions in ion flux dynamics for different modulation frequencies and at the startup of the plasma were analyzed together with intensified charge coupled device images recording the plasma propagation in order to assess the dynamics of plasma plume propagation and how it is impacted by ‘memory effects’. Quantitative measurements of the ion densities enabling these memory effects are reported. The results in this paper highlight the tremendous impact of memory effects on plasma propagation and the corresponding pre-ionization.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Kinetic Modeling Analysis of Ar Addition to Atmospheric Pressure N 2 –H 2 Plasma for Plasma-Assisted Catalytic Synthesis of NH 3

Zero-dimensional kinetic modeling of atmospheric pressure Ar–N 2 –H 2 nonthermal plasma was carried out to gain mechanistic insights into plasma-assisted catalytic synthesis of ammonia. Ar dilution is a common technique for tailoring plasma discharge properties and has been shown to enhance NH 3 formation when added to N 2 –H 2 plasma. The kinetic model was developed for a coaxial dielectric barrier discharge quartz wool-packed bed reactor operating at near room temperature using a kHz-frequency plasma source. With 30% Ar mixed in a 1:1 N 2 –H 2 plasma at 760 Torr, we find that NH 3 production is dominated by Eley–Rideal (E-R) surface reactions, which heavily involve surface NH x species derived from N and H radicals in the gas phase, while the influence of excited N 2 molecules is negligible. This is contrary to the commonly proposed mechanism that excited N 2 molecules created by Penning excitation of N 2 by Ar(4s) and Ar(4p) play a significant role in assisting NH 3 formation. Our model shows that the enhanced NH 3 formation upon Ar dilution is unlikely due to the interactions between Ar and H species, as excited Ar atoms have a weak effect on H radical formation through H 2 dissociation compared to electrons. We find that excited Ar atoms contribute to 28% of the N radical production in the gas phase via N 2 dissociation, while the rest are dominated by electron-impact dissociation. Furthermore, Ar species play a negligible role in the product NH 3 dissociation. N 2 conversion sensitivity analyses were carried out for electron number density (ne) and reduced electric field (E/N), and contributions from Ar to gas-phase N radical production were quantified. Finally, the model can provide guidance on potential reasons for observing enhanced NH 3 formation upon Ar dilution in N 2 –H 2 plasma beyond changes in the discharge characteristics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Constraining the destruction rate of K 40 in stellar nucleosynthesis through the study of the Ar 40 ( p , n ) K 40 reaction

Background: We present that K 40 plays a significant role in the radiogenic heating of Earth-like exoplanets, which can affect the development of a habitable environment on their surfaces. The initial amount of K 40 in the interior of these planets depends on the composition of the interstellar clouds from which they formed. Within this context, nuclear reactions that regulate the production of K 40 during stellar evolution can play a critical role. Purpose: In this study, we constrain for the first time the astrophysical reaction rate of K 40 ( n , p ) Ar 40 , which is responsible for the destruction of K 40 during stellar nucleosynthesis. We provide to the nuclear physics community high-resolution data on the cross section and angular distribution of the Ar 40 ( p , n ) K 40 reaction. These are important to various applications involving Ar 40 . The associated reaction rate of the Ar 40 ( p , n ) K 40 process addresses a reaction rate gap in the Joint Institute for Nuclear Astrophysics REACLIB database in the region of intermediate-mass isotopes. Methods: We performed differential cross-section measurements on the Ar 40 ( p , n ) K 40 reaction, for six energies in the center-of-mass system between 3.2 and 4.0 MeV and various angles between 0 ° and 135 ° . The experiment took place at the Edwards Accelerator Laboratory at Ohio University using the beam swinger target location and a standard neutron time-of-flight technique. We extracted total and partial cross sections by integrating the double differential cross sections we measured. Results: The total and partial cross sections varied with energy due to the contribution from isobaric analog states and Ericson type fluctuations. The energy-averaged neutron angular distributions were symmetrical relative to 90 ° . Based on the experimental data, local transmission coefficients were extracted and were used to calculate the astrophysical reaction rates of Ar 40 ( p , n ) K 40 and K 40 ( n , p ) Ar 40 reactions. The new rates were found to vary significantly from the theoretical rates in the REACLIB library. We implemented the new rates in network calculations to study nucleosynthesis via the slow neutron capture process, and we found that the produced abundance of K 40 is reduced by up to 10% compared to calculations with the library rates. At the same time, the above result removes a significant portion of the previous theoretical uncertainty on the K 40 yields from stellar evolution calculations. Conclusions: Our results support a destruction rate of K 40 in massive stars via the K 40 ( n , p ) Ar 40 reaction that is larger compared to previous estimates. The rate of K 40 destruction via the K 40 ( n , p ) Ar 40 reaction now has a dramatically reduced uncertainty based on our measurement. Lastly, this result directly affects the predicted stellar yields of K 40 from nucleosynthesis, which is a critical input parameter for the galactic chemical evolution models that are currently employed for the study of significant properties of exoplanets.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Subsurface cosmogenic and radiogenic production of 42 Ar

Radioactive decays from 42 Ar and its progeny 42 K are potential background sources in large-scale liquid-argon-based neutrino and dark matter experiments. In the atmosphere, 42 Ar is produced primarily by cosmogenic activation on 40 Ar. The use of low radioactivity argon from cosmogenically shielded underground sources can expand the reach and sensitivity of liquid-argon-based rare event searches. We estimate 42 Ar production underground by nuclear reactions induced by natural radioactivity and cosmic-ray muon-induced interactions. At 3,000 mwe, 42 Ar production rate is 1.8×10 -3 atoms per ton of crust per year, 7 orders of magnitude smaller than the 39 Ar production rate at a similar depth in the crust. In conclusion, by comparing the calculated production rate of 42 Ar to that of 39 Ar for which the concentration has been measured in an underground gas sample, we estimate the activity of 42 Ar in gas extracted from 3,000 mwe depth to be less than two decays per ton of argon per year.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Dynamics of argon metastables in Ar–CH 4 radio frequency capacitively-coupled plasma: real-time monitoring with neural network-augmented broadband optical emission spectroscopy

In moderate-pressure radio frequency (RF) capacitively coupled plasmas generated in argon–methane mixtures, the density of argon metastable atoms (Ar 1 s 5 ) exhibits a non-monotonic dependence on methane (CH 4 ) concentration. Laser-induced fluorescence (LIF) was used to measure and compare local Ar 1 s 5 densities in Ar and Ar–CH 4 plasmas at 2.6 Torr and RF powers of 17–117 W. The addition of 1% CH 4 increases the metastable density, and 2% CH 4 triggers a strong depletion by an order of magnitude, compared to 1% CH 4 case. This non-monotonic behavior demonstrates the sensitivity of metastable populations to small gas admixtures, which is critical for processes where metastables drive precursor dissociation. For real-time monitoring of metastable population, broadband optical emission spectroscopy (OES) is augmented with a feedforward neural network (NN) to predict Ar s1 5 densities from spectral features. When trained on LIF data, the NN replicates the absolute densities and the dynamic trends of Ar 1 s 5 density variation. The NN-augmented broadband OES approach can be used as a simple and cost-effective tool for tracking Ar metastables in Ar-rich plasmas, facilitating industrial-scale optimization.

Yatom, Shurik [Princeton Plasma Physics Laboratory↗