First experimental determination of the 40Ar( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si13.svg" display="inline" id="d1e1637"> <mml:mrow> <mml:mi>n</mml:mi> <mml:mo>,</mml:mo> <mml:mn>2</mml:mn> <mml:mi>n</mml:mi> </mml:mrow>
The cosmogenic $^{39}$Ar(t$_{1/2}$= 268 years) isotope of argon is used for geophysical dating and tracing owing to its appropriate half-life and chemical inertness as a noble gas; $^{39}$Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main $^{39}$Ar cosmogenic production reaction in the atmosphere, namely $^{40}$Ar$(n,2n)^{39}$Ar, using 14.8$\pm0.3$ MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the $^{40}$Ar isotope. The reaction yield was measured by atom counting of $^{39}$Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon. A total $^{40}$Ar$(n,2n)^{39}$Ar cross section of 610$\pm100$ mb was determined. 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 $^{39}$Ar atmospheric production, resulting in $770\pm240$ $^{39}$Ar atoms/cm$^2$/day. The secular equilibrium between the $^{39}$Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance $^{39}$Ar/Ar$= (5.9\pm 1.8) \times 10^{-16}$, showing that $\approx$73% of atmospheric $^{39}$Ar is produced by cosmogenic neutrons. The $^{40}$Ar($n,2n$)$^{39}$Ar 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 $^{39}$Ar accounts for roughly 20% of the present atmospheric inventory.
Authors
- Adam M. Clark (ORCID: https://orcid.org/0000-0002-2881-7982)
- D. Neto (ORCID: https://orcid.org/0000-0002-5397-7048)
- M. Tessler (ORCID: https://orcid.org/0000-0002-8935-4555)
- R. C. Pardo (ORCID: https://orcid.org/0000-0002-8264-9430)
- Toralf Döring
- Κ. Zuber (ORCID: https://orcid.org/0000-0001-8689-4495)
- Marie Pichotta (ORCID: https://orcid.org/0009-0009-1917-7870)
- S. Bhattacharya (ORCID: https://orcid.org/0009-0009-3660-8396)
- Austin Nelson (ORCID: https://orcid.org/0000-0002-4253-6837)
- Lauren Callahan (ORCID: https://orcid.org/0000-0001-5548-2084)
- D. Bemmerer (ORCID: https://orcid.org/0000-0003-0470-8367)
- Rudra N. Sahoo (ORCID: https://orcid.org/0000-0002-9405-9542)
- R. Schwengner (ORCID: https://orcid.org/0000-0002-7620-8882)
- Roland Purtschert (ORCID: https://orcid.org/0000-0002-4734-7664)
- Thomas L. Bailey
- C. Ugalde (ORCID: https://orcid.org/0000-0003-2721-6728)
- R. Scott (ORCID: https://orcid.org/0000-0001-7032-9264)
- I. Tolstukhin (ORCID: https://orcid.org/0000-0002-6631-7479)
- Y. Kashiv (ORCID: https://orcid.org/0000-0002-5989-8789)
- M. L. Avila (ORCID: https://orcid.org/0009-0002-4051-9627)
- P. Collon
- K. E. Rehm
- Chloé Fougères (ORCID: https://orcid.org/0000-0002-1236-4739)
- E. López-Saavedra (ORCID: https://orcid.org/0000-0001-9187-0404)
- Hans F. R. Hoffmann (ORCID: https://orcid.org/0009-0004-3188-6569)
- Jonathan E. Dickerson
- D. Robertson (ORCID: https://orcid.org/0000-0002-4961-1641)
- M. Paul (ORCID: https://orcid.org/0000-0002-4121-8597)
- J. McLain (ORCID: https://orcid.org/0000-0002-5584-5436)
- R. Vondrasek (ORCID: https://orcid.org/0000-0003-0862-3897)
- S. Vaintraub
Publication Details
- Journal
- Geochimica et Cosmochimica Acta
- Published
- 2025-12-19
- DOI
- https://doi.org/10.1016/j.gca.2025.12.041
- Citations
- 1
- Primary Topic
- Radioactive contamination and transfer
- Type
- article
- Field-Weighted Citation Impact
- 1.11