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30Si Mole Fraction of a Silicon Material Highly Enriched in 28Si Determined by Instrumental Neutron Activation Analysis

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 Publication date 2016
  fields Physics
and research's language is English




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The latest determination of the Avogadro constant, carried out by counting the atoms in a pure silicon crystal highly enriched in 28Si, reached the target 2x10-8 relative uncertainty required for the redefinition of the kilogram based on the Planck constant. The knowledge of the isotopic composition of the enriched silicon material is central; it is measured by isotope dilution mass spectrometry. In this work, an independent estimate of the 30Si mole fraction was obtained by applying a relative measurement protocol based on Instrumental Neutron Activation Analysis. The amount of 30Si isotope was determined by counting the 1266.1 keV gamma-photons emitted during the radioactive decay of the radioisotope 31Si produced via the neutron capture reaction 30Si(n,gamma)31Si. The x(30Si) = 1.043(19)x10-6 mol mol-1 is consistent with the value currently adopted by the International Avogadro Coordination.



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The determination of the Avogadro constant plays a key role in the redefinition of the kilogram in terms of a fundamental constant. The present experiment makes use of a silicon single-crystal highly enriched in 28Si that must have a total impurity mass fraction smaller than a few parts in 109. To verify this requirement, we previously developed a relative analytical method based on neutron activation for the elemental characterization of a sample of the precursor natural silicon crystal WASO 04. The method is now extended to fifty-nine elements and applied to a monoisotopic 28Si single-crystal that was grown to test the achievable enrichment. Since this crystal was likely contaminated, this measurement tested also the detection capabilities of the analysis. The results quantified contaminations by Ge, Ga, As, Tm, Lu, Ta, W and Ir and, for a number of the detectable elements, demonstrated that we can already reach the targeted 1 ng/g detection limit.
We investigated the use of neutron activation to estimate the 30Si mole fraction of the ultra-pure silicon material highly enriched in 28Si for the measurement of the Avogadro constant. Specifically, we developed a relative method based on Instrumental Neutron Activation Analysis and using a natural-Si sample as a standard. To evaluate the achievable uncertainty, we irradiated a 6 g sample of a natural-Si material and modeled experimentally the signal that would be produced by a sample of the 28Si-enriched material of similar mass and subjected to the same measurement conditions. The extrapolation of the expected uncertainty from the experimental data indicates that a measurement of the 30Si mole fraction of the 28Si-enriched material might reach a 4% relative combined standard uncertainty.
The production of $^{3}$H, $^{7}$Be, and $^{22}$Na by interactions of cosmic-ray particles with silicon can produce radioactive backgrounds in detectors used to search for rare events. Through controlled irradiation of silicon CCDs and wafers with a neutron beam that mimics the cosmic-ray neutron spectrum, followed by direct counting, we determined that the production rate from cosmic-ray neutrons at sea level is ($112 pm 24$) atoms/(kg day) for $^{3}$H, ($8.1 pm 1.9 $) atoms/(kg day) for $^{7}$Be, and ($43.0 pm 7.1 $) atoms/(kg day) for $^{22}$Na. Complementing these results with the current best estimates of activation cross sections for cosmic-ray particles other than neutrons, we obtain a total sea-level cosmic-ray production rate of ($124 pm 24$) atoms/(kg day) for $^{3}$H, ($9.4 pm 2.0 $) atoms/(kg day) for $^{7}$Be, and ($49.6 pm 7.3 $) atoms/(kg day) for $^{22}$Na. These measurements will help constrain background estimates and determine the maximum time that silicon-based detectors can remain unshielded during detector fabrication before cosmogenic backgrounds impact the sensitivity of next-generation rare-event searches.
In this paper we present Monte Carlo N-Particle (MCNP) simulations of the system for underwater threat detection using neutron activation analysis developed in the SABAT project. The simulated system is based on a D-T neutron generator emitting 14~MeV neutrons without associated $alpha$ particle detection and equipped with a LaBr$_3$:Ce scintillation detector offering superior energy resolution and allowing for precise identification of activation $gamma$ quanta. The performed simulations show that using the neutron activation analysis method with the designed geometry we are able to identify $gamma$-rays from hydrogen, carbon, sulphur and chlorine originating from mustard gas in a sea water environment. Our results show that the most efficient way of mustard gas detection is to compare the integral peak ratio for Cl and H.
The Advanced Molybdenum-based Rare process Experiment in its second phase (AMoRE-II) will search for neutrinoless double-beta (0{ u}b{eta}b{eta}) decay of 100Mo in 200 kg of molybdate crystals. To achieve the zero-background level in the energy range of the double-beta decay Q-value of 100Mo, the radioactive contamination levels in AMoRE crystals should be low. 100EnrMoO3 powder, which is enriched in the 100Mo isotope, is used to grow the AMoRE crystals. A shielded array of fourteen high-purity germanium detectors with 70% relative efficiency each was used for the measurement of background activities in a sample of 9.6-kg powder. The detector system named CAGe located at the Yangyang underground laboratory was designed for measuring low levels of radioactivity from natural radioisotopes or cosmogenic nuclides such as 228Ac, 228Th, 226Ra, 88Y, and 40K. The activities of 228Ac and 228Th in the powder sample were 0.88 pm 0.12 mBq/kg and 0.669 pm 0.087 mBq/kg, respectively. The activity of 226Ra was measured to be 1.50 pm 0.23 mBq/kg. The activity of 88Y was 0.101 pm 0.016 mBq/kg. The activity of 40K was found as 36.0 pm 4.1 mBq/kg.
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