The analysis and attribution of the time-dependent neutron background resultant from sample irradiation in a SLOWPOKE-2 reactor

The Royal Military College of Canada (RMCC) has commissioned a Delayed Neutron Counting (DNC) system for the analysis of special nuclear materials. A significant, time-dependent neutron background with an initial maximum count rate, more than 50 times that of the time-independent background, was characterised during the validation of this system. This time-dependent background was found to be dependent on the presence of the polyethylene (PE) vials used to transport the fissile samples, yet was not an activation product of vial impurities. The magnitude of the time-dependent background was found to be irradiation site specific and independent of the mass of PE. The capability of RMCC’s DNC system to analyze the neutron count rates in time intervals <1 s facilitated a more detailed data analysis than that obtained in previous DNC systems recording cumulative neutron counts. An analysis of the time-dependent background behaviour suggested that an equivalent of 120 ng of ²³⁵U contamination was present on each irradiated vial. However, Inductively Coupled Plasma—Mass Spectroscopy measurements of material leached from the outer vial surfaces after their irradiations found only trace amounts of uranium, 0.118 ± 0.048 ng of ²³⁵U derived from natural uranium. These quantities are insufficient to account for the time-independent background, and in fact could not be discriminated from the noise associated with time-independent background. It is suggested that delayed neutron emitters are deposited in the vial surface following fission recoil, leaving the main body of uranium within the irradiation site. This hypothesis is supported by the physical cleaning of the site with materials soaked in distilled water and HNO₃, which lowered the background from a nominal ²³⁵U mass equivalent of 120 to 50 ng per vial.     

Optimum timing parameters in 14 MeV neutron activation analysis of thorium and uranium using delayed neutron counting

A detailed theoretical treatment of cyclic activation analysis of thorium and uranium using a 14 MeV neutron generator and delayed neutron counting is presented. Variations of the detector response with sample transfer and total experiment times are examined in order to obtain the optimum cycle periods for the maximum detector response. Cycle optimization for 95% and 90% of the maximum detector response is investigated. Furthermore, elimination of the delayed neutrons produced by the reaction¹⁷O(n,p)¹⁷N is also considered in optimum cycle timing. Finally, calculations are carried out to estimate detection limits for thorium and uranium. Experimental results will be reported in a subsequent paper.     

On-stream nuclear activation of trace uranium and thorium using a 14 MeV neutron generator

A method for the continuous on-stream determination of trace concentrations of uranium and thorium in flowing streams is developed. The 14 MeV neutron generator was used for irradiation and the delayed neutron counting technique was employed in counting the induced neutron activity. The dependence of the minimum detectable concentration on the irradiation, decay and counting times, liquid flow-rate and the background was studied. At optimal conditions, uranium and thorium concentrations were determined down to 20 and 100 ppm, respectively. The interference of the neutron emitting nuclide^17m O was reduced to an insignificant level by optimizing the decay time.     

Oxygen determination by fast neutron activation

A method for the determination of oxygen based on the reaction¹⁶O(n, p)¹⁶N is suggested. The samples are irradiated in stainless steel capsules with fast neutrons. The total neutron flux passing through the sample is proportional to the flux passing through the wall of the capsule. Therefore, the activity induced in the capsule according to the reaction⁵⁶Fe(n, p)⁵⁶Mn can be used to monitor the neutron flux through the sample. Thus, the necessity of maintaining the sample in an exact position during the irradiation is eliminated.     

Analysis of uranium using delayed neutron emission

Analyses of uranium and thorium by delayed neutron counting are described.The experimental system comprises an automatic pneumatic transfer system associatedwith a device made of twelve BF 3 neutron counters. Using homogeneous preparedsolutions of the samples, the analyses were based on a triple cycle each including60-second irradiation followed by 1-second cooling and 60-second counting.In these conditions, the limit of detection of uranium is about 0.3 µgwith a precision of measurement better than 10%. The contributions of possibleperturbations from 17 O(n,p)17 N reactions, followed by simultaneous –disintegration and neutron emission and from (n) reactions, have been studied.     

Neutron activation analysis of uranium in human bone,drinking water and daily diet

Uranium in human bone, drinking water and daily diet has been determined by neutron activation analysis using the²³⁸U(n, γ)²³⁹U reaction. An improved scheme for the separation of the²³⁹U is proposed; with this scheme, after neutron irradiation in a 100 kW TRIGA reactor, a uranium content as low as 5·10⁻¹¹ g can be determined reliably, rapidly and easily. A wide range of uranium concentrations, from about 0.1 ppb up to about 10 ppb has been found in the bones of normal Japanese. Water from several Japanese city water services, and the daily diet taken in two Japanese cities, have been found to contain an average 9·10⁻⁹ g/l and 1.5 μg per person-day uranium, respectively.     

Evaluation of New Pharmaceuticals Using In Vivo Neutron Inelastic Scattering and Neutron Activation Analysis

Nutritional status of patients can be evaluated by monitoring changes in body composition, including depletion of protein and muscle, adipose tissue distribution and changes in hydration status, bone or cell mass. Fast neutron activation (for N and P) and neutron inelastic scattering (for C and O) are used to assess in vivo elements characteristic of specific body compartments. The fast neutrons are produced with a sealed deuterium-tritium (D-T) neutron generator. This method provides the most direct assessment of body composition. Non-bone phosphorus for muscle is measured by the ³¹P(n,)²⁸Al reaction, and nitrogen for protein via the (n,2n) fast neutron reaction. Inelastic neutron scattering is used for the measurement of total body carbon and oxygen. Carbon is used to derive body fat, after subtracting carbon contributions due to protein, bone and glycogen. Carbon-to-oxygen (C/O) ratio is used to measure distribution of fat and lean tissue in the body and to monitor small changes of lean mass and its quality. In addition to evaluating the efficacy of new treatments, the system is used to study the mechanisms of lean tissue depletion with aging and to investigate methods for preserving function and quality of life in the elderly.     

Studies of Low-Frequency Molecular Motions in Polymers by Neutron Inelastic Scattering

Abstract

The energy distribution of a monoenergetic incident neutron beam after a single scattering event provides information concerning the molecular motions of a polymer in the region 800 to 30 cm^?1. In polyethylene (Marlex 6050) several peaks are observed in the neutron spectrum between 200 and 600 cm^?1. The frequencies corresponding to these peaks are in good agreement with those predicted from a calculation of the dispersion relations of the skeletal modes (bending and stretching) taking into account interchain forces. In the case of an oriented sample of the polymer, a polarization effect can be obtained by placing the momentum transfer K of the neutron parallel or perpendicular to the chain direction S. This allows the identification of transverse and longitudinal modes of vibration. This effect has been studied in the case of polyethylene and polyoxymethylene. The frequency distribution of phonons, derived from the neutron data under certain approximations, were also obtained from samples of polyoxymethylene, polyacrylonitrile, and polyethylene glycol. These results are compared with the observed infrared and the calculated frequencies.     

Neutron activation analysis for ultra low contents of uranium and thorium in aluminium and silica

Highly sensitive neutron activation analysis of uranium and thorium in high quality silica and aluminium has been investigated using the Japan Materials Testing Reactor (JMTR), having a thermal neutron flux higher than 10¹⁴ n/cm²/s. In order to determine ultra-low contents of uranium and thorium,²³⁹Np and²³³Pa as activation products were separated by using anion exchange and LaF₃ coprecipitation methods. As a result, a number of interfering radioactive isotopes containing double neutron capture product such as¹⁸³Ta were removed completely from the isolated²³⁹Np and²³³Pa fraction and the detection limits for uranium and thorium were found to be 2·10^–12 g and 4·10^–13 g, respectively.     

Etude de la reaction 14N(d.n)15O a basse energie et application au dosage de l'azote dans le zirconium

Study of the ¹⁴N(d,n)¹⁵O reaction at low energy and application to the determination of nitrogen in zirconiumThe thick target yield for the ¹⁴N(d,n)¹⁵O reaction weis determined between 1 MeV and 5.5 MeV; the “average energy” and the sensitivity of the analysis for nitrogen are calculated. Nitrogen can be determined in zirconium samples at the level of 35 μg g^?1, by irradiating at 4 MeV and 5.5 MeV in a deuteron beam from a Van de Graaff accelerator. After irradiation, the samples are subjected to reducing fusion in a graphite crucible, to separate ¹⁵O. The results are compared with those obtained by other methods on identical samples; there is a difference of 3–17%.     

Feasibility of using dendroanalysis of uranium as a biomarker for environmental contamination

A study was initiated to investigate the chronological deposition of uranium in certain species of trees growing on the site of a former uranium metal processing facility. The Feed Materials Production Center (FMPC) is located in Fernald, Ohio, and for roughly 40 years operated as a large scale uranium processing center. Core samples from several species of trees growing in different locations throughout the site were extracted using a 12.5 mm incremental wood boring drill bit. After extraction, each core sample was cut and packaged into individual sections representing 4 annual growth rings and submitted for instrumental neutron activation analysis (INAA). The reaction ²³⁵U(n,f)¹⁴⁰Ba→¹⁴⁰La+γ was evaluated using high resolution germanium gamma-spectroscopy to detect the 1.596 MeV photon emission from the fission product ¹⁴⁰La following a minimum of a 3 week decay. A total of 106 samples representing 7 individual trees of 3 unique species were irradiated. In addition to the tree-core samples, 18 quality control (QC) samples and 18 standard reference material (SRM) Fly Ash samples were irradiated with the core samples for determining neutron flux. The activity in any one sample in a batch was determined by comparison with the amount of natural uranium in the QC standards. No significantly measurable amount of uranium was detected in any of the tree core samples, although 3 tree core samples were in excess of the minimum detectable amount (30 ng).     

Neutron activation method for nitrogen determination in biological specimens

For the determination of the nitrogen content in plants, 14 MeV neutron activation analysis was used based on the determination of the elemental concentration by measuring the area of the gamma-radiation of the radionuclide¹³N as a result of¹⁴N(n, 2n)¹³N reaction. Three methods were tested in order to obtain quantitative results: comparator method, method for absolute determination of the neutron flux and monitor method. Using the monitor method, results for nitrogen content in plant species were obtained-for beans 74.8% and for maize 1.8%. The precision of determination is ±10%. The possible sources of errors are analyzed. The efficiency of the Ge(Li) detector has been determined using a combined -source in the energy interval 120–1400 keV with precision of 4.5%. The sensitivity achieved was 4 mg or 47 imp/mg per min.     

Neutron activation analysis of ivory of African elephants

Instrumental neutron activation analysis was applied to 80 samples from various African countries and 81 samples from the Kruger National Park in the Republic of South Africa. Twelve elements such as Br, Ca, Cl, Co, Cs, Fe, Mg, Mn, Na, Sc, Sr, and Zn, were determined in all samples. The factor scores of each sample were calculated from those elemental concentrations for the first and second factors to clarify the differences of samples from various African countries with those from Kruger Park. The results were compared with those by stable isotope analysis (¹³C and¹⁵N).     

Neutron activation analysis with PE moderated252Cf neutron source

The 1.369 MeV -rays emitted from²⁴Na²⁴Mg+^–+ after²³Na(n,)²⁴Na reaction were counted by high purity germanium (HPGe) detector and the half-life of²⁴Na was derived. This process was simulated by Monte Carlo Neutron and Photon Transport Code (MCNP-4A).²⁵²Cf neutron source was moderated by a polyethylene (PE) cylinder to increase the cross section of neutron absorption reaction and to decrease the biological hazard. NaCl powder of 20 cm³ and 40 cm³ volume in cylindrical polypropylene capsules were irradiated by the neutrons passed through the moderator. MCNP-4A was used to determine the optimum size of PE moderator, to assume the realistic geometry of the HPGe detector, and to assume the absolute efficiencies of the detector. The count rates for 1.369 MeV -rays in the HPGe detector were calculated by MCNP-4A for 20 cm³ and 40 cm³ NaCl. The accumulated counts calculated tumed out to be higher than those actually measured by 31% with a relative error of 3%. The half-life of²⁴Na measured within 4% and 1% for 20 cm³ and 40cm³ NaCl agrees with that of the reference. So, we can say that the result of MCNP-4A has about 30% of accuracy and 3% of precision in simulating the neutron activation analysis.     

Neutron activation analysis of ivory of African elephants

Instrumental neutron activation analysis was applied to 61 ivory samples of which origin countries are known. 12 elements such as Br, Ca, Cl, Co, Cs, Fe, Mg, Mn, Na, Sc, Sr and Zn, were determined in all samples. The factor score of each sample was calculated for each factor by making use of principal component analysis in order to determine their origins. The results were compared with those by stable isotope analysis (¹³C and¹⁵N).     

Neutron captue prompt gamma-ray activation analysis at the NIST Cold Neutron Research Facility

An instrument for neutron capture prompt gamma-ray activation analysis (PGAA) has been constructed as part of the Cold Neutron Research Facility at the 20 MW National Institute of Standards and Technology Research Reactor. The neutron fluence rate (thermal equivalent) is 1.5·10⁸ n ·cm^–2·s^–1, with negligible fast neutrons and gamma-rays. With compact geometry and hydrogen-free construction, the sensitivity is sevenfold better than an existing thermal instrument. Hydrogen background is thirtyfold lower.     

Neutron self-shielding in hydrogenous samples

Measurements performed in the past to determine sensitivity enhancements (later identified as neutron density increases) in PGNAA as a function of hydrogen concentration in slab-shaped samples are described. The results are compared to the results of Monte Carlo computations. It is concluded that, like H₂O, D₂O can also cause substantial neutron density increases. In one concentrated salt solution, however, D₂O seems to cause a neutron density decrease that cannot be explained from the macroscopic neutron scattering and absorption cross sections in the model used.     

New method to measure oxygen isotopic concentration ratios18O/16O by gamma-activation analysis,especially in biological media

The photonuclear reactions used for this isotopic analysis are as follows:¹⁶O(γ, n)¹⁵O threshold energy 15.7 MeV;¹⁸O(γ, p)¹⁷N threshold energy 16.3 MeV.¹⁵O is a pure β⁺ emitter of half-life 2.03 minutes, whereas¹⁷N presents a 4.2 second neutron emission. The principle of the method is founded on the simultaneous measurement of the above characteristic radioactivities, the intensities of which are proportional to the respective quantities of¹⁶O and¹⁸O present in the irradiated sample. The potentialities of this new oxygen isotope analysis method, based on the use of an electron accelerator, are described. Detection limit of 0.1 μg¹⁸O is easily attainable. The equipment designed and built to industrialise this technique is described. It allows a hundred samples to be analysed automatically, the accelerator, detection instruments and pneumatic transfer circuits being controlled by a logic system linked to an electronic chronometer.     

Neutron activation analysis of rare earth impurities in metallic uranium

A method with a sensitivity of 2·10⁻⁷ to 1·10⁻¹⁰% has been developed for determining Yb, Ho, Dy, Gd, Eu, Sm and La impurities in metallic uranium by means of neutron activation. The method is based on a preliminary chromatographic separation of the total amount of rare earth elements from uranium by passing the solution in sulphuric acid through KU-2 cation exchange resin and eluting the traces of uranium retained by the resin with a solution of ascorbic acid. The rare earth impurities are then eluted from the resin with 4–5N HCl, evaporated, and irradiated for 20 hours with a neutron flux of 1.2·10¹³ n·cm⁻²·sec⁻¹. Subsequently the traces of the rare earth elements are co-precipitated with Fe(OH)₃, dissolved in concentrated HCl and separated from the iron and other impurities by passing the solution through Dowex 1X8 anion exchange resin in the chloride form. The individual rare earth elements are then separated from each other using KU-2 cation exchange resin and a solution of ammonium α-hydroxyisobutyrate as the eluant.     

The application of NAA with irradiation at reduced temperature for the study of element losses during pretreatment of biological samples

The neutron capture gamma-ray spectroscopy facility assembled at the Institute of Radiochemistry, KfK (for analytical purposes) using a²⁵²Cf neutron source with a strength of 6·10⁷ n/s, has been used to check its applicability and sensitivity for quantitative analyses of ores. The analysis of Sm, Cd and Mn in phosphate and monazite rock samples has been carried out. The results from this study show a variation of about 25% from the values determined by RNAA method. This discrepancy could be mainly due to the low signal-to-background ratio observed which is caused by (i) scattering of the source gammarays by the target, and (ii) interference from the 2223.1 keV neutron capture hydrogen gamma-rays produced by the moderated materials and from their compton scattering in the detector. To overcome these difficulties we suggest to introduce a 2.5 cm thick polyethylene sheet between the detector⁶Li-cap shielding and the target as well as to increase the detection solid angle. Also the strength of the²⁵²Cf neutron source should be increased by an order of magnitude and the neutron beam should be collimated to obtain the optimal thermal neutron flux with a low level of²⁵²Cf gamma-rays. This can be achieved by setting up between the neutron source and the target a conical polyethylene collimator with a thickness of 10 cm containing a 1 cm thick lead sheet.