Analysis of marine samples by neutron-induced prompt gamma-ray technique and ICP-MS

Multi-element and isotopic analyses of oils and marine environmental samples were carried out to estimate a contamination source using a "finger printing" method. Elemental analyses were carried out using neutron-induced prompt gamma-ray analysis (PGA), instrumental neutron activation analysis (INAA) at the Japan Atomic Energy Research Institute, Tokai-mura, Japan (JAERI) and ICP-MS in the IAEA Marine Environment Laboratory, Monaco (MEL). Fifteen elements including light elements, H, B, N, Si and Ca, which cannot be determined by INAA and ICP-MS, were determined by PGA. A total of 47 elements were determined in the present study. The potential of PGA for the determination of isotopic ratios was tested by measuring ³⁴S/³²S ratios in oils. The evaluation of historical records of marine environmental conditions using annual bands in coral samples was also investigated.     

Determination of boron in Japanese geochemical reference samples by neutron-induced prompt gamma-ray analysis

Determination of ppm levels of B in 21 igneous and sedimentary rocks of the Japanese geochemical reference samples prepared by the Geological Survey of Japan (GSJ) has been performed by neutron-induced prompt γ-ray analysis (PGA) using cold and thermal guided neutron beams of the JRR-3M. Owing to the Doppler broadened γ-ray line of B 478 keV, many elements such as Na, Ni, Cl and so on showed spectral interference in the determination of B. The interference was corrected by computer fitting and a reference peak method. The analytical results obtained by the present method almost agreed with the GSJ values recommended in 1994 within the standard deviation of the recommended values. Sodium contents determined by the PGA in the reference rock samples are also reported.     

Multi-element analysis of environmental samples by cold and thermal guided neutron induced prompt gamma-ray measurement

Non-destructive multi-element determination in environmental samples by neutron-induced prompt -ray analysis (PGA) has been investigated. Comparative standardization for the elements including H, B, C, N, Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, Mn, Fe, Co, Cd, Sm, Gd, Hg by PGA has been carried out using the cold and thermal guided neutron beams of JRR-3M reactor and then several environmental reference materials have been analyzed. Accuracy and precision of better than 20% were found for these elemental analyses except for H, C, N and Cl in biological samples. Detection limits in various environmental matrices were 25 to 820 ng/g for B, Cd, Sm and Gd, 1.1 to 820 g/g for H, Na, S, Cl, K, Ti, Mn, Co and Hg, and 0.031 to 10% for C, N, Mg, Al, Si, P, Ca and Fe. The present method is being applied to environmental studies of post war Persian Gulf together with INAA and ICP-MS.     

Application of low background gamma-ray spectrometry to environmental monitoring samples: Water leaching treatment for 40K-removal

In the usual measurements of radionuclides in the environmental samples by g-ray spectrometry, Compton scattering of 1461 keV g-rays from ⁴⁰K severely interferes with the detection of artificial radionuclides in marine and agricultural products. In order to eliminate the interference of ⁴⁰K, we have developed a simple and convenient water leaching treatment method applicable to seaweed (sargasso) samples. By this treatment, over 98% of the potassium in seaweed samples is removed without notable losses of artificial and/or natural radionuclides. In combination with the low-level g-ray counting in the Ogoya underground laboratory, the detection limit could be improved by ~1 order of magnitude.     

Reliability of prompt gamma-ray analysis for the determination of Na and Mg in rock samples.

The reliability of neutron-induced prompt gamma-ray analysis (PGA) was examined for the determination of Na and Mg in geological and cosmochemical rock samples, because they tend to have been erroneously determined for such samples. JB-1 (basalt standard rock) and Allende (chondritic meteorite) powder samples were repeatedly analyzed by using thermal or cold neutron-guided beams of the JRR-3M research reactor at Japan Atomic Energy Agency. In critically evaluating calculated values for major prompt gamma-rays of Na and Mg, it was observed that a 472.2 keV peak for Na and a 2828.2 keV peak for Mg yielded reasonable consistency with corresponding recommended values. Sodium and Mg were determined for five lunar meteorites by PGA using these prompt gamma-rays, and were found to be consistent with their data obtained by instrumental neutron activation analysis.     

Thickness Determination of Ultra-Thin Films on Si Substrates by EPMA

Results from thickness determination of single-element ultra-thin (<10nm) films by electron probe microanalysis (EPMA) are presented. The studied samples were Ge, Sn, Ag and Au thin films deposited by resistive evaporation on Si substrates. The thickness of the films was controlled during evaporation by means of a quartz crystal, previously calibrated using samples with overlayers of different thicknesses (>20nm) measured by Rutherford backscatter spectrometry and optical interferometry. EPMA measurements were performed on an electron microprobe CAMECA SX-50, with incident electron energies ranging from 4keV to 20keV. Film thicknesses were derived from the measured k-ratios using the analytical programs X-Film and Layerf and the Monte Carlo simulation code Penelope. The ionization cross sections used in the simulations were calculated with the distorted-wave Born approximation. Film thicknesses obtained from the EPMA measurements using the various computational methods are compared with those measured with the quartz crystal. The maximum relative difference between results from the different techniques does not exceed 5%.     

Boron in coral skeletons determined by prompt γ-ray analysis

A systematic and non-destructive technique is proposed for the determination of boron in coral samples by neutron-induced prompt γ-ray analysis (PGA) using a thermal neutron guide beam of the JRR-3M reactor. About 50–150 mg samples in sealed FEP film were irradiated and measured for 5000 s in the PGA system at a neutron flux of 2.4 × 10⁷ n cm⁻² s⁻¹. In order to determine B content in coral skeletons, the Doppler-broadened γ-ray peak of 478 keV (¹⁰B) was used together with the correction of interference from the Na-peak of 472 keV. The analytical precision was ~3% for the JCp-1 coral standard. The data (n = 56) obtained by the present method showed a range of B content from 40.7 to 76.9 ppm which is similar to reported values. Boron in corals showed the highest levels in Rukan-sho (Okinawa) with an average B content of 62.5 ppm, whereas corals collected from Mizugama (Okinawa), Cebu (the Philippines) and Khang Khao (Thailand) exhibited B contents of 56.5, 53.0 and 45.7 ppm, respectively. The uptake of boron by living corals may be influenced by seawater pH related to higher seawater B(OH)₄⁻. In this paper we discuss factors controlling the B levels in corals.     

Uranium and thorium determination in Brazilian coals by epithermal neutron activation analysis

An experimental technique has been developed to determine impurities in coal. Uranium was determined by counting the²³⁹Np 106.1 keV -ray with a LEPS detector and thorium by counting the²³³Pa 311.8 keV -ray with a Ge(Li) detector. Seventeen coal samples were analyzed with an average precision of 3% and a quantitative determination limit of 0.153 g/g for uranium and 0.078 g/g for thorium. The technique allows determinations of up to twenty elements besides U and Th and can be applied in routine analysis.     

Variation of the Kβ/Kα intensity ratios of Ti, V and Cr in halogen compounds versus excitation energy in the interval 5.5-12.1 keV

The K/K intensity ratios for Ti, V and Cr in halogen (F and Cl) compounds were investigated. Measurements were carried out at ten different energies in the 5.5-12.1 keV interval by using the secondary excitation method. K X-rays emitted by the samples were counted by a Si(Li) detector with a resolution of 160 eV at 5.9 keV. It was observed that the measured values are getting closer to the theoretical values with increasing excitation energy. Values obtained were compared with the theoretical ones for pure elements.     

Determination of boron in glass by alpha-spectrometry

Alpha-spectrometric method has been used for the determination of boron in borosilicate glasses. For irradiation thermal neutrons with a flux of about 10⁵ n·cm^–2·s^–1, produced in a paraffin moderator surrounding a deuteron target of a small neutron generator, were used. Alpha-particles from the reaction¹⁰B(n, ) were detected by a Si solid state detector with a resolution of about 50 keV. The sensitivity of the method is 0.05 wt % boron in glass samples.This work was supported by the Hungarian Research Foundation (Contract No. 1734/91.).     

A practical approach for self-absorption correction in210Pb gamma-spectrometric dating

Self-absorption correction of low-energy (<100 keV) -radiation is a much debated subject when applying low-energy -rays for dating purposes. Some investigations have hitherto focused on the possibility of using either irradiating of the sample and subsequent absortiometry or introducing physical correction. In the present paper an automatic procedure was elaborated using the occurrences of other low-energy -lines in the sample, those of²³⁴Th. Theoretical considerations are described on the basis of the mass absorption coefficients as a function of energy and atomic number. These considerations are verified by experiments with rock forming oxides and carbonates mixed with Standard Reference Material. Finally, an example is given for the application of the self-absorption correction approach.     

Gamma-spectrometric determination of uranium isotopes in biofuel ash

Gamma-ray measurements have been performed on biofuel samples using a planar intrinsic Ge detector. The samples were first homogenized and then packed into 90 ml plastic tubs. The radiation from each sample was usually measured for 1 to 2 days. The intensity of the 63.3 keV -ray in²³⁴Th was used to determine the amount of²³⁸U present. The amount of²³⁵U can be determined from the intensity of the 143.8 keV -ray.     

Distribution of137Cs,40K,238U and232Th in soils from Northern Venezuela

More than one hundred undisturbed soil samples from Northern Venezuela and the islands of Margarita and Los Roques have been analyzed for¹³⁷Cs,⁴⁰K,²³⁸U and²³²Th by -ray spectroscopy. The specimens were taken from between 5–10 cm below the earth's surface. Thus, they are valid not only for the¹³⁷Cs deposition studies but also for the estimation of the natural -ray dose from primordial radionuclides that form the terrestrial component. The concentration of⁴⁰K was directly determined from its 1461 keV -ray, while those of¹³⁷Cs,²³⁸U and²³²Th were performed using a -ray from one of their daughter radionuclides: the 661 keV -ray of^137mBa for¹³⁷Cs, the 1760 keV -ray of²¹⁴Bi for²³⁸U and the 2620 keV -ray of²⁰⁸Tl for²³²Th. Finally, the concentration values were compared with those of global estimates.     

Determination of neptunium in plutonium and mixed uranium-plutonium samples by isotope dilution gamma-spectrometry with243Am as a spike

A method was developed for isolating neptunium from Pu, U or mixed oxide (MOX) samples and its determination by isotope dilution -spectrometry (IDGS) using²³⁹Np (²⁴³Am) as a spike. Extraction chromatography with trilaurylamine fixed on a SGX-C18 support was used for the isolation of Np. The decontamination factors for U, Pu, Am and Pa vary between 1000–2000 and 100, respectively. The average separation yield of Np is (95±3)%. The amount of²⁴³Am required for spiking is about 0.2–0.3 g. It is recommended to use the pair of -rays 86.53 keV (²³⁷Np)-106.13 keV (²³⁹Np) for the assay of neptunium. A relative uncertainty of 4% or better is achievable in the analysis of plutonium samples, containing 0.4–80 g neptunium. The detection limit, under the proposed experimental conditions, is about 0.05 g Np. The results were compared with the results obtained by using high resolution -spectrometry (HRGS).     

The measurement of “enhanced” L and M X-ray yields from charge-induced studies with protons and1H 2 + ion beams

Earlier work on Charge Induced X-rays (CHIX) was extended to include the X-ray energy region between 0.70 to 4.0 keV. Protons of 700 keV, and¹H ₂ ⁺ ion beams of equivalent proton energies in the range 350–450 keV were used to produce enhanced yields of L and MX-rays from a suitable selection of highly compacted non-conducting samples. Enhancement factors are given and possible applications are mentioned.     

Simultaneous radiochemical determination of237Np and239Np with235Np as a tracer,and application to environmental samples

Neptunium is sorbed, together with plutonium, uranium and iron on Bio Rad AG 1×4 anion exchange resin from 9 mol/1 HCl, eluted with 7 mol/l HNO₃ and 1.2 mol/l HCl, purified on a second, identical column and electrodeposited on stainless steel discs.²³⁷Np is determined by -spectrometry,²³⁹Np by -spectrometry with a Ge detector, or via its 14.3 keV LX-rays in a Si(Li) measurement. The neptunium yield is determined from the count rate of the 13.6 keV LX rays of the tracer²³⁵Np in a later Si(Li) measurement. The average chemical yield is 78±11%. The detection limit for²³⁷Np is 1 mBq. The procedure allows the sequential determination of neptunium, together with plutonium, strontium, uranium and iron from one sample. The method was applied to air and total deposition samples from Munich-Neuherberg and to sediment samples from the Irish sea.     

The study of sensitivity and resolution of microautoradiography using Auger electrons

By using low energy beta emitter to microautoradiography, it is expected that high resolution microautoradiogram can be made. In this report, the authors pay attention to the use of monochromatic and low energy electron on the metallic samples, and used⁵¹Cr that emits Auger electrons with the energy of 4.5keV and⁶⁵Zn that emits Auger electrons with energy of 7keV in the study of the resolution of Auger electron microautoradiograph. From the results of the study, it was clearly confirmed that the resolution of the microautoradiograph using⁵¹Cr was better than 0.5 m and the resolution using⁶⁵Zn was better than 1 m.In order to make high resolution microautoradiograph, it is essentially important to know the sensitivity of the nuclear emulsion to the low energy electrons in advance, for securing the reasonable exposure to the nuclear emulsion. In this regard, the investigation on the sensitivities of those emulsions to the Auger electrons with the energy of 5.4keV from⁵⁵Fe and 7keV from⁶⁵Zn was made using Ilford and Fuji nuclear emulsions.     

Heat Resistance and Local Structure of FeCl2-Absorbed Crosslinked Poly(γ-Glutamic Acid)

Fiber of Japanese food natto (Bacillus subtilis) is known to be superabsorbent poly(-glutamic acid) (PGA). NaCl particles precipitate in FeCl₂-absorbed crosslinked PGA when heated at crystallization temperature of 320 °C for 10 to 60 min. After heat treatment the Mössbauer spectrum of FeCl₂-crosslinked PGA consists of a quadrupole doublet due to FeCl₂·2H₂O. The Mössbauer spectrum of anhydrous FeCl₂ reagent heated under the same condition shows an intense sextet due to -Fe₂O₃ . These results prove that the superabsorbent polymer, crosslinked PGA, has higher heat resistance.     

Crystalline Inclusions Formed in C+N+BF2 Coimplanted on Silicon (111)

In the present work, high-doses (10¹⁷–10¹⁸cm^–2) of carbon, nitrogen, and boron (BF₂⁺) ions were coimplanted on silicon (111) substrates at 21, 25 and 77keV, respectively. Two series of samples have been implanted (series A and B) and subsequently annealed. Series A samples have been implanted at room temperature and treated one minute by rapid thermal annealing (RTA) and 3 hours at 1200°C. Series B samples have been implanted at 600°C and subsequently annealed at 1200°C during 3 hours. The annealing in both series has been carried out in N₂ at atmospheric pressures.The structure of the buried layers has been determined by conventional and high resolution transmission electron microscopy (CTEM and HRTEM). Polycrystalline silicon and new crystalline phases are observed by electron diffraction patterns. The polycrystalline silicon inclusions have been confirmed from analysis of HRTEM images.     

Determination of137Cs and134Cs in air samples collected near Belgrade /Yugoslavia/ following the Chernobyl accident

This paper presents the results of measurements of¹³⁷Cs and¹³⁴Cs content in air sampled during May 1986. Maximum concentrations:¹³⁷Cs 2.94±0.01 Bq m^–3 and¹³⁴Cs 1.38±0.01 Bq m^–3 were registered on May 3. Several other long lived radionuclides having -energies in the region 33 keV to 1365 keV were registered in the same samples two years later. The results of measurements of the total -activity in air for the same period are also presented.