Tracer Applications of Noble Gas Radionuclides in the Geosciences

The noble gas radionuclides, including 81Kr (half-life = 229,000 yr), 85Kr (11 yr), and 39Ar (269 yr), possess nearly ideal chemical and physical properties for studies of earth and environmental processes. Recent advances in Atom Trap Trace Analysis (ATTA), a laser-based atom counting method, have enabled routine measurements of the radiokrypton isotopes, as well as the demonstration of the ability to measure 39Ar in environmental samples. Here we provide an overview of the ATTA technique, and a survey of recent progress made in several laboratories worldwide. We review the application of noble gas radionuclides in the geosciences and discuss how ATTA can help advance these fields, specifically determination of groundwater residence times using 81Kr, 85Kr, and 39Ar; dating old glacial ice using 81Kr; and an 39Ar survey of the main water masses of the oceans, to study circulation pathways and estimate mean residence times. Other scientific questions involving deeper circulation of fluids in the Earth's crust and mantle also are within the scope of future applications. We conclude that the geoscience community would greatly benefit from an ATTA facility dedicated to this field, with instrumentation for routine measurements, as well as for research on further development of ATTA methods

Quantification of 37Ar emanation fractions from irradiated natural rock samples and field applications.

Underground-produced 37Ar can be used for underground nuclear explosions (UNE) detection and for groundwater dating. The quantification of the emanation, that is the fraction of activity produced in the rock that escapes to the pore space, is essential for predicting the background activity expected in natural environments. We propose an experiment in which artificial CaCO3 powder and natural rock particles are irradiated with neutrons in a routinely operated medical cyclotron, whose energy spectrum is experimentally measured. The produced activity was quantified and compared with the emanated activity to determine the emanating fraction. The results showed consistent and reproducible patterns with a dominance of the recoil process at small scales (<2 mm). We observed emanation values ≤1% with a dependency on the grain size and the inner geometry of particles. Soil weathering and the presence of water increased the recoil emanation. The atoms produced that were instantaneously recoiled in the intra- or inter-granular pore space left macroscopic samples by diffusion on timescales of days to weeks (Deff = 10-12 - 10-16 m2 s-1). This diffusive transport determines the activity that prevails in the fluid-filled pore space accessible for groundwater or soil gas sampling

A New Method of Measuring 81Kr and 85Kr Abundances in Environmental Samples

We demonstrate a new method for determining the 81Kr/Kr ratio in environmental samples based upon two measurements: the 85Kr/81Kr ratio measured by Atom Trap Trace Analysis (ATTA) and the 85Kr/Kr ratio measured by Low-Level Counting (LLC). This method can be used to determine the mean residence time of groundwater in the range of 10^5 - 10^6 a. It requires a sample of 100 micro-l STP of Kr extracted from approximately two tons of water. With modern atmospheric Kr samples, we demonstrate that the ratios measured by ATTA and LLC are directly proportional to each other within the measurement error of +/- 10%; we calibrate the 81Kr/Kr ratio of modern air measured using this method; and we show that the 81Kr/Kr ratios of samples extracted from air before and after the development of the nuclear industry are identical within the measurement error

Operational Experience with a Cryogenic Axial-Centrifugal Compressor

The Large Hadron Collider (LHC), presently under construction at CERN, requires large refrigeration capacity at 1.8 K. Compression of gaseous helium at cryogenic temperatures is therefore inevitable. Together with subcontractors, Linde Kryotechnik has developed a prototype machine. This unit is based on a cryogenic axial-centrifugal compressor, running on ceramic ball bearings and driven by a variable-frequency electrical motor operating at ambient temperature. Integrated in a test facility for superconducting magnets the machine has been commissioned without major problems and successfully gone through the acceptance test in autumn 1995. Subsequent steps were initiated to improve efficiency of this prototype. This paper describes operating experience gained so far and reports on measured performance prior to and after constructional modifications

Ar-39 Detection at the 10^-16 Isotopic Abundance Level with Atom Trap Trace Analysis

Atom Trap Trace Analysis (ATTA), a laser-based atom counting method, has been applied to analyze atmospheric Ar-39 (half-life = 269 yr), a cosmogenic isotope with an isotopic abundance of 8x10^-16. In addition to the superior selectivity demonstrated in this work, counting rate and efficiency of ATTA have been improved by two orders of magnitude over prior results. Significant applications of this new analytical capability lie in radioisotope dating of ice and water samples and in the development of dark matter detectors

Atmospheric 81Kr as an integrator of cosmic-ray flux on the hundred-thousand-year timescale

The atmospheric abundance of 81Kr is a global integrator of cosmic rays. It is insensitive to climate shifts, geographical variations, and short-term solar cycle activity, making it an ideal standard to test models of cosmic-ray flux on the time scale of 105 years. Here we present the first calculation of absolute 81Kr production rates in the atmosphere, and a measurement of the atmospheric 81Kr/Kr abundance via the Atom Trap Trace Analysis method. The measurement result significantly deviates from previously reported values. The agreement between measurement and model prediction supports the current understanding of the production mechanisms. Additionally, the calculated 81Kr atmospheric inventory over the past 1.5 Myr provides a more accurate input function for radiokrypton dating

Ar39 Detection at the 10\u3csup\u3e-\u3c/sup\u3e16 Isotopic Abundance Level with Atom Trap Trace Analysis

Atom trap trace analysis, a laser-based atom counting method, has been applied to analyze atmospheric Ar39 (half-life=269yr), a cosmogenic isotope with an isotopic abundance of 8×10-16. In addition to the superior selectivity demonstrated in this work, the counting rate and efficiency of atom trap trace analysis have been improved by 2 orders of magnitude over prior results. The significant applications of this new analytical capability lie in radioisotope dating of ice and water samples and in the development of dark matter detectors. © 2011 American Physical Society

Stellar 36,38^{36,38}Ar(n,γ)37,39(n,\gamma)^{37,39}Ar reactions and their effect on light neutron-rich nuclide synthesis

The $^{36}$Ar$(n,\gamma)^{37}$Ar ($t_{1/2}$ = 35 d) and $^{38}$Ar$(n,\gamma)^{39}$Ar (269 y) reactions were studied for the first time with a quasi-Maxwellian ($kT \sim 47$ keV) neutron flux for Maxwellian Average Cross Section (MACS) measurements at stellar energies. Gas samples were irradiated at the high-intensity Soreq applied research accelerator facility-liquid-lithium target neutron source and the $^{37}$Ar/$^{36}$Ar and $^{39}$Ar/$^{38}$Ar ratios in the activated samples were determined by accelerator mass spectrometry at the ATLAS facility (Argonne National Laboratory). The $^{37}$Ar activity was also measured by low-level counting at the University of Bern. Experimental MACS of $^{36}$Ar and $^{38}$Ar, corrected to the standard 30 keV thermal energy, are 1.9(3) mb and 1.3(2) mb, respectively, differing from the theoretical and evaluated values published to date by up to an order of magnitude. The neutron capture cross sections of $^{36,38}$Ar are relevant to the stellar nucleosynthesis of light neutron-rich nuclides; the two experimental values are shown to affect the calculated mass fraction of nuclides in the region A=36-48 during the weak $s$-process. The new production cross sections have implications also for the use of $^{37}$Ar and $^{39}$Ar as environmental tracers in the atmosphere and hydrosphere.Comment: 18 pages + Supp. Mat. (13 pages) Accepted for publication in Phys. Rev. Let

Rapid processing of ⁸⁵5 Kr/Kr ratios using Atom Trap Trace Analysis

We report a methodology for measuring ⁸⁵ Kr/Kr isotopic abundances using Atom Trap Trace Analysis (ATTA) that increases sample measurement throughput by over an order of magnitude to six samples per 24 h. The noble gas isotope ⁸⁵ Kr (half-life 510.7 years) is a useful tracer for young groundwater in the age range of 5–50 years. ATTA, an efficient and selective laser-based atom counting method, has recently been applied to ⁸⁵ Kr/Kr isotopic abundance measurements, requiring 5–10 μL of krypton gas at STP extracted from 50 to 100 L of water. Previously, a single such measurement required 48 h. Our new method demonstrates that we can measure 85Kr/Kr ratios with 3–5% relative uncertainty every 4 h, on average, with the same sample requirements