Design considerations for a neutron generator-based total-body irradiator

Summary The prompt- and delayed-gamma neutron activation techniques have been used for the non-invasive measurement of human body composition. In recent years, neutron irradiators have used only transuranic isotopic sources (^{238PuBe, 241}AmBe, ²⁵²Cf). However, in today’s security-minded environment, the use of alternate neutron sources may provide some advantages. We have examined several designs for an irradiator that would use a high-output, miniature D-T neutron generator (MF Physics). The use of this type of neutron source will lessen the storage, security, and transport issues associated with continuous-output isotopic neutron sources. To determine the scientific impact of this decision, we have performed Monte Carlo simulations (MCNP-4B2; Los Alamos National Laboratory) to aid in the design of the irradiator system, evaluating shielding materials, collimation, and source-to-subject distance, for the measurement of total body nitrogen (TBN). Based on internal flux distributions within the simulated body region of a subject, several design options were identified. The final design will be selected based on the optimization of precision, dose, and exposure time.     

Non-destructive determination of trace amounts of iodine in biological samples by epithermal neutron activation and Compton suppression gamma-ray spectrometry

In order to investigate the ingestion of iodine by human body and to know its content in organs, instrumental epithermal neutron activation analysis was used in conjunction with Compton suppression gamma-ray spectrometry by measuring the ¹²⁸I short-lived nuclide. The interferences of ²⁴Na and ³⁸Cl induced from NaCl in a sample were reduced by factors of about 6 and 15 to 41 by employing the epithermal neutron activation and Compton suppression gamma-ray spectrometry, respectively. The present method can be used to determine iodine at levels higher than 11 ppb. It was applied to the determination of iodine of more than 35 ppb in various biological reference materials.     

Determination of human and Sprague-Dawley rat trimethylselenonium ion and total selenium urine concentrations from endogenous body selenium pool by neutron activation analysis

This study determined trimethylselenonium ion [TMSe, (CH₃)₃Se⁺] and total organic selenium cationic species urinary excretion values for healthy human subjects and Sprague-Dawley rats fed regular diets. The only source of TMSe was from the endogenous selenium body pool. Total selenium concentration, in urine was determined by instrumental neutron activation analysis. TMSe and total selenium cationic species concentrations and percent of total selenium urine excretion were determined by chemical neutron activation analysis and coupled anion-cation exchange chromatography and anion-exchange chromatography, respectively. Within experimental error, mean values for TMSe and cationic species as percent selenium were comparable for both human subjects and Sprague-Dawley rats. This study suggested that TMSe excreted in urine by healthy human subjects and Sprague-Dawley rats fed a normal diet is not a minor but a general metabolite of selenium ingested in a normal diet.     

Postmortem activation analysis: Preliminary observations in the preterm infant

Few data exist on the elemental composition of the human body during infancy. The scarcity of the data is due, in part, to the destructive nature of total body analyses normally required for the classical chemical approach. To help determine such data for infants, we have developed a neutron activation facility for nondestructive postmortem analyses. The system consists of a multisource²⁴¹AmBe irradiator and a multidetector NaI(T1) whole body counter. The total body contents of K, Ca, P, Na and Cl are determined. Postmortem examinations have been performed in twelve infant cadavers. These results are compared with those of the reference fetus.     

Determination of232Th in human tissues by pre-concentration neutron activation analysis with yield determination using227Th

The accurate and precise determination of²³²Th in biological samples is very important for the development of biokinetic models for thorium and for improving our knowledge on its distribution in human tissues. Radiochemical neutron activation analysis has long been one of the most sensitive methods for the determination of²³²Th. However, these determinations suffer in reliability because recovery information following the separation is not typically available. This information is particularly important for difficult matrices such as human bone where recoveries may be significantly less than unity. Also, the separation of difficult matrices following neutron activation may involve relatively high personal dose from the co-activated matrix. A novel approach for the determination of radiochemical yield has been developed which employs the use of a readily available, gamma-emitting isotope of thorium,²²⁷Th.²²⁷Th, obtained by radiochemical separation from²²⁷Ac, is added to each, dissolved sample prior to separation and the chemical yield determined by gamma-ray spectrometry following the separation. This pre-concentration step is then followed by neutron activation and the²³²Th determined via²³³Pa using gamma-ray spectrometry. Detection limits were approximately an order of magnitude lower than obtained by alpha-spectrometry.     

The determination of selenium in water samples from the environment

A method for the determination of selenium by preconcentration and thermal neutron activation is presented. Selenium is adsorbed on active charcoal after reduction to the elemental state. By varying the conditions of the reduction, it is possible to measure the total selenium content and tetravalent selenium separately. The contribution of hexavalent selenium is obtained by substraction. The lower limit of determination is 5 ng°1⁻¹. About 40 samples per day can be handled by one analyst. The preconcentration can be performed at the sampling site resulting in samples, which can be stored easily for later analyses by neutron activation.     

Actinides and Long-Lived Radionuclides in Tissues of the Japanese Population: Summary of the Past 20-Year Studies

Radioactive fallout constitutes the major source of contamination of the environment with fission products. Our primary interest was in selected fission products, such as ¹³¹I, ⁸⁹Sr, ⁹⁰Sr, and ¹³⁷Cs, and neutron activation products, such as ³H and ¹⁴C. Plutonium-239,240, ²⁴¹Am and ⁹⁰Tc are generated from nuclear tests, and they are important by-products of nuclear industries. Polonium-210, ²¹⁰Pb and ²³²Th, ²³⁰Th and ²²⁸Th occur widely in nature. These radionuclides enter the human body through inhalation and the ingestion through food and water. These nuclides may cause radiation doses to certain organs of the body. Assessment of the resulting health hazards is an essential public health activity, which demands reliable techniques for the assay of the various radionuclides in man and his environment. In this paper, we present the accumulation of radionuclides from man-made sources and primordial radionuclides in various tissues of the Japanese population. The studies were performed at the Department of Public Health, Akita University School of Medicine, during the periods from 1973 to 1995.     

Evolution of 40K in fruit collected in Malaysia by the determination of total potassium using neutron activation analysis

Potassium is an extremely important major to element to the human body. Potassium in made up of three isotopes with abundances of ³⁹K at 93.1%, ⁴⁰K at 0.0118% and ⁴¹K at 6.88%. It is also very well known that ⁴⁰K is to measure the single 1460.8 keV photon from beta-decay. However, this procedure requires a significant amount of sample and typical counting periods of at least a day in well-shielded germanium counting system. Another approach is to determination total potassium via neutron activation analysis using the well know ⁴¹K (n,γ) ⁴²K(T _1/2 = 12.8 h) reaction and then evaluate ⁴⁰K using the usual activity equation A = λN. In our laboratory we have effectively used thermal and epithermal neutron flux for neutron activation analysis to determine potassium in fruits. Upward to 7–9 batches of samples, which each of batch is including 14 samples so can be analysed in 1 day using only gram quantities of material. In such way on can increase the output of determining ⁴⁰K by at least on order of magnitude. Result of a detailed investigation optimization of the methodology, quality control and detection limits will be presented for reference material and various fruits samples.     

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.     

Use of D–T-produced fast neutrons for in vivo body composition analysis: a reference method for nutritional assessment in the elderly

Body composition has become the main outcome of many nutritional intervention studies including osteoporosis, malnutrition, obesity, AIDS, and aging. Traditional indirect body composition methods developed with healthy young adults do not apply to the elderly or diseased. 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. Non-bone phosphorus for muscle is measured by the ³¹P(n,)²⁸Al reaction, and nitrogen for protein via the ¹⁴N(n,2n)¹³N fast neutron reaction. Inelastic neutron scattering is used to measure total body carbon and oxygen. Body fat is derived from carbon after correcting for contributions from protein, bone, and glycogen. Carbon-to-oxygen ratio (C/O) is used to measure the distribution of fat and lean tissue in the body and to monitor small changes of lean mass. A sealed, D–T neutron generator is used for the production of fast neutrons. Carbon and oxygen mass and their ratio are measured in vivo at a radiation exposure of less than 0.06 mSv. Gamma-ray spectra are collected using large BGO detectors and analyzed for the 4.43 MeV state of carbon and 6.13 MeV state of oxygen, simultaneously with the irradiation. P and N analysis by delayed fast neutron activation is performed by transferring the patient to a shielded room equipped with an array of NaI(Tl) detectors. A combination of measurements makes possible the assessment of the quality of fat-free mass. The neutron generator system is used to evaluate the efficacy of new treatments, to study mechanisms of lean tissue depletion with aging, and to investigate methods for preserving function and quality of life in the elderly. It is also used as a reference method for the validation of portable instruments of nutritional assessment.     

Small sample in-vivo neutron activation analysis using californium sources

This work describes an in vivo neutron activation analysis facility for small samples, such as rats or human hand, using two 100 g²⁵²Cf neutron sources. The irradiation area is a cylindrical space, of 12 cm diameter and about 15 cm length, with fairly uniform neutron flux distribution. Experimental data on the reproducibility, effects of volume and other conditions for in vivo measurements are given. Comparative atomic absorption data on calcium measurements on rats are reported. The facility is now used for animal experiments as well as human hand irradiations in clinical investigations involving calcium metabolism and bone diseases.     

Sol particle immunoassays using colloidal gold and neutron activation

The feasibility of performing immunoassays with colloidal gold labels and detection of¹⁹⁸Au by neutron activation has been demonstrated with measurements of human immunoglobulin and of serum antibodies to human immunodeficiency virus type 1. The detection sensitivity achieved after activation in a high flux reactor or with a water moderated²⁵²Cf source, by gamma-counting or by autoradiography, is similar to the sensitivity obtained with absorbance measurements in the more common enzyme immunoassays. The reactor based neutron activation assay allows detection of 10^–16 mol of analyte in routine operation with possible extension to 10^–20 mol. The sensitivity with the 1.3 Ci²⁵²Cf source is limited to about 10^–15 mol. The practical limitations of the assay's sensitivity at this point are due to background signals from reagents and/or nonspecific binding of the gold labeled reagent.     

Measurements of the photonuclear neutron yield of 15 MV medical linear accelerator

High energy medical linear accelerators (>10 MV) are increasingly used in radiotherapy. At such high photon energies neutron production via photonuclear reactions in the heavy elements which compose the linac head is inevitable. Neutrons from linacs can contribute to an additional dose to staff, patients and the general public. Our intention is two-fold; to provide shielding against the neutron contamination and to establish the depthdose curve of thermal neutrons within human tissue, with an aim to utilise linacs in boron neuron capture therapy (BNCT). In our studies neutron measurements were undertaken, with a Varian Clinac 2100C/D linear accelerator operating at 15 MV nominal energy, by irradiating 18 cm thick 30×30 cm² block of tissue equivalent material. Measurements were taken using indium and aluminum activation foil at the centre of the block. Our results show that by leaving the linac jaws open neutron production is increased compared to the case when these are shut, for one minute exposure at 400MU. In this work we present a comparison between our results and existing literature and attempt to explore some sharp contrasts.     

Research reactors as sources of atmospheric radioxenon

Radioxenon emissions of the TRIGA Mark II research reactor in Vienna were investigated with respect to a possible impact on the verification of the Comprehensive Nuclear Test-Ban-Treaty. Using the Swedish Automatic Unit for Noble Gas Acquisition (SAUNA II), five radioxenon isotopes ¹²⁵Xe, ^131mXe, ^133mXe, ¹³³Xe and ¹³⁵Xe were detected, of which ¹²⁵Xe is solely produced by neutron capture in stable atmospheric ¹²⁴Xe and hence acts as an indicator for neutron activation processes. The other nuclides are produced in both fission and neutron capture reactions. The detected activity concentrations ranged from 0.0010 to 190 Bq/m³. The source of the radioxenon is not yet fully clarified, but it could be micro-cracks in the fuel cladding, fission of ²³⁵U contaminations on the outside of the fuel elements or neutron activation of atmospheric Xe. Neutron deficient ¹²⁵Xe with its highly complex decay scheme was seen for the first time in a SAUNA system. In many experiments the activity ratios of the radioxenon nuclides carry the signature of nuclear explosions, if ^131mXe is omitted. Only if ^131mXe is included into the calculations of the isotopic activity ratios, the majority of the measurements revealed a “civil” signature (typical for a NPP). A significant contribution of the TRIGA Vienna to the global or European radioxenon inventory can be excluded. Due to the very low activities, the emissions are far below any concern for human health.     

Evaluation of 40K in food by determining total potassium using neutron activation analysis

Summary Potassium is an extremely important major element to the human body. Potassium is made up of three isotopes with abundances of ³⁹K at 93.1%, ⁴⁰K at 0.0118% and ⁴¹K at 6.88%. It is also very well known that ⁴⁰K with its 1.3 ^. 10⁹ years half-life is a major naturally occurring isotope in the body and food. The usual way to determine total ⁴⁰K is to measure the single 1460.8 keV photon from beta-decay. However, this procedure requires a significant amount of sample and typical counting periods of at least a day in well-shielded germanium counting system. Another approach is to determine total potassium via neutron activation analysis using the well known ⁴¹K(n,g)⁴²K (T_1/2 = 12.8 h) reaction and then evaluate ⁴⁰K using the usual activity equation A = lN. In our laboratory we have effectively used epithermal neutron activation analysis and Compton suppression to determine potassium in air filters and other geological material. Upwards to 10-15 samples can be analyzed in one day using only gram quantities of material. In such way one can increase the output of determining ⁴⁰K by at least one order of magnitude. Results of a detailed investigation optimization of the methodology, quality control and detection limits will be presented for reference material and various food samples.     

Determination of129I and127I in human thyroid blocks containing mercury as a preservative

A solvent extraction techniques has been developed to separate iodine from mercury contained in thyroid tissues for the determinations of¹²⁹I and¹²⁷I in human thyroid blocks by neutron activation analysis. The tissue samples are digested with a mixture of 5 ml HCl and 1 ml HNO₃ in a round-bottomed flask fitted with a condenser running with cold water to avoid any loss of iodine. Iodine is extracted into 0.1 M dihexyl sulfide solution in xylene leaving the majority of the mercury in the aqueous phase. Iodine is adsorbed on activated charcoal packed in quartz tubes either by heating the xylene containing iodine in the presence of oxygen or by heating the aqueous solution obtained after back extracting iodine from xylene using a saturated sulfur dioxide solution. Iodine is desorbed from the charcoal and trapped into a quartz ampule which is sent for neutron activation.     

Biomedical neutron research at the Californium User Facility for Neutron Science

The Californium User Facility for Neutron Science has been established at Oak Ridge National Laboratory (ORNL). The Californium Use Facility (CUF) is a part of the larger Californium Facility, which fabricates and stores compact²⁵²Cf neutron sources for worldwide distribution. The CUF can provide a cost-effective option for research with²⁵²Cf sources. Three projects at the CUF that demonstrate the versatility of²⁵²Cf for biological and biomedical neutron-based research are described: future establishment of a²⁵²Cf-based neutron activation analysis system, ongoing work to produce miniature high-intensity, remotely afterloaded²⁵²Cf sources for tumors therapy, and a recent experiment that irradiated living human lung cancer cells impregnated with experimental boron compounds to test their effectiveness for boron neutron capture therapy.     

Arsenic distribution in rats fed a Hijiki diet

Very large doses of sodium arsenate (Na₂HAsO₄), 14 mg As kg^?1 of body weight, were administered to Sprague-Dawley male rats (body weight 300 g) fed a 5% Hijiki diet by stomach tube twice within two days. After 24 h, the rats were sacrificed and various organs were dried for subsequent neutron activation analysis. The distribution of arsenic (As) in selected organs was determined by neutron activation analysis. The highest concentration of As was found in blood cells with a rather high concentration in the liver and heart. As the control, rats which were fed on a 5% cellulose diet were used. Control rats which were administered arsenate showed that the arsenic distribution and the concentration in their organs were similar to those on the 5% Hijiki diet. Even the blood cells of the controls without any arsenic administration were found to contain a small amount of arsenic.     

Determination of uranium element concentration and235U isotope abundance by neutron activation analysis

A new neutron activation technique has been developed for the determination of uranium element concentration and²³⁵U isotope abundance in nuclear safeguards and reference material samples based on the activation of bare and cadmium-covered samples with different thermal to epithermal neutron flux ratios and on the combination of the two corre-sponding delayed-fission neutron measurements. The principle of the new technique can be applied also to improve multi-element neutron activation analysis.     

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.