Rapid analysis of trinitite with nuclear forensic applications for post-detonation material analyses

Analysis of post-nuclear detonation materials provides information on the type of device and its origin. Compositional analysis of trinitite glass, fused silicate material produced from the above ground plasma during the detonation of the Trinity nuclear bomb, reveals gross scale chemical and isotopic heterogeneities indicative of limited convective re-homogenization during accumulation into a melt pool at ground zero. Regions rich in weapons grade Pu have also been identified on the surface of the trinitite sample. The absolute and relative abundances of the lanthanoids in the glass are comparable to that of average upper crust composition, whereas the isotopic abundances of key lanthanoids are distinctly non-normal. The trinitite glass has a non-normal Nd isotope composition, with deviations of ?1.75 ± 0.60 ε (differences in parts in 10⁴) in ¹⁴²Nd/¹⁴⁴Nd, +2.24 ± 0.75 ε in ¹⁴⁵Nd/¹⁴⁴Nd, and +1.01 ± 0.38 ε in ¹⁴⁸Nd/¹⁴⁴Nd (all errors cited at 2σ) relative to reference materials: BHVO-2 and Nd-Ames metal. Greater isotopic deviations are found in Gd, with enrichments of +4 ± 1 ε in ¹⁵⁵Gd/¹⁶⁰Gd, +4.19 ± 0.75 ε in ¹⁵⁶Gd/¹⁶⁰Gd, and +3.48 ± 0.52 ε in ¹⁵⁸Gd/¹⁶⁰Gd compared to BHVO-2. The isotopic deviations are consistent with a ²³⁹Pu based fission device with additional ²³⁵U fission contribution and a thermal neutron fluence between 1.4 and 0.97 × 10¹⁵ neutrons/cm².     

Correction of k<Subscript>0</Subscript>-factors for non-1/v elements based on neutron spectrum measurements

Neutron spectra were measured by the time of flight method using a rotating disk chopper system in the JRR-3M prompt gamma ray analysis system. Effective g-factors for non-1/v elements such as Cd, Sm and Gd were calculated from the measured neutron spectra and the neutron cross section data, and they was used for correcting the k ₀-factors. The resulting k ₀-factors for the cold and thermal neutron beams agreed within 10%. Furthermore, the prompt gamma ray emission probabilities of Cd, Sm and Gd were derived from the corrected k ₀-factors using other relevant physical constants.     

Neutron spectrum correction of k0-factors for k0-based neutron-induced prompt gamma-ray analysis

Neutron spectrum correction has been attempted for the k₀-factors of the non-1/v elements which are affected neutron spectrum difference. Effective g-factors and Westcott g-factors, which are neutron spectrum correction factors obtained from an actual neutron spectrum and the Maxwellian distribution, respectively, for the non-1/v elements were calculated using their neutron cross section data of JENDEL-3.2. The neutron spectrum correction was made for the measured k₀-factors of the non-1/v elements such as Cd, Sm and Gd with the cold and thermal guided neutron beams of JRR-3M using the g-factors. The corrected k₀-factors between the cold and thermal neutron beams using both g-factors for both neutron beams agreed well for Cd. However, 9 to 44% deviations have been found for Sm and Gd, respectively.     

Production of a <Superscript>173</Superscript>Lu target for neutron capture cross section measurements

Lutetium has been used as a radiochemistry detector to measure neutron fluence in NTS tests. A measure of the neutron capture cross sections on ¹⁷³Lu is needed to improve the interpretation value of the Lu radiochemistry isotopic ratios. A natural hafnium target was irradiated with protons to produce neutron poor lutetium radioisotopes. The short lived species were allowed to decay prior to chemical processing resulting in predominantly ¹⁷³Lu with a small amount of ¹⁷⁴Lu. This material was deposited on a titanium foil for use in the neutron capture cross section measurement.     

INAA determination of holmium in submilligram samples of cosmochemical and geochemical interest and the second-order activation interference

Second-order neutron activation becomes a serious interference in NAA determinations of REE in submilligram samples of meteoritic and terrestrial materials when neutron fluences reach levels of 10²⁰ n·cm^–2 or more. The Dy-interference to Ho determination and the Eu-interference to Gd determination are quite, large. We discuss the importance of second-order activation interferences in REE determinations, and present an experimental method to correct the Dy-interference to Ho determination by INAA. Ho concentrations in splits of less than 0.2 mg of BCR-1 and SP can be accurately determined by INAA with a neutron fluence of 2·10²⁰ n·cm^–2 in spite of large Dy interferences of up to 200%. It is necessary for NAA determinations of REE with high neutron fluences that each REE standard be separated from its neighboring REE, in order to correct the second-order activation interferences experimentally.     

Preparation of radio-Sm by neutron activation for accelerator mass spectrometry

Field measurement of isotopic ratios may be used to fingerprint an element’s origin, be it from commercial power, industrial, medical or historical weapons fallout. Samples of samarium radionuclides were prepared by neutron activation for subsequent analysis using accelerator mass spectrometry (AMS). High purity samarium (III) oxide powder was irradiated in the University of Texas at Austin TRIGA reactor to a total neutron fluence of 5 × 10¹⁵ cm^?2. An initial determination of the isotopic ratios was made using activation calculations with a BURN card in an MCNPX-based model of the TRIGA core. Experimental validation of the MCNP results was achieved by analyzing gamma spectra of the irradiated oxide powers after irradiation. Subsequent measurement of ¹⁵¹Sm will be conducted at the CAMS facility at LLNL demonstrating the first measurement of this isotope at this facility.     

Investigation of fast neutron shielding characteristics depending on boron percentages of MgB<Subscript>2</Subscript>, NaBH<Subscript>4</Subscript> and KBH<Subscript>4</Subscript>

The macroscopic cross-section Σ and average neutron fluence in matter Φ are usable factors to comment neutron shielding property of samples. In this paper, we have used MgB₂, NaBH₄ and KBH₄ samples including different percentages of boron. Neutron macroscopic cross-section measurements of them have been done by using a source of mono-energetic neutrons (E _eff = 4.5 MeV ²⁴¹Am–Be). Average neutron fluence values and double differential fast neutron flux distributions of each samples calculated by using FLUKA Monte Carlo code. Also half value layers (HVLs) of samples are compared to paraffin which is one of the most neutron moderators. As a result, growing boron concentration can raise neutron shielding property of materials.     

Precise determination of cadmium and lead isotopic compositions in river sediments

A method for the accurate determination of Cd and Pb isotope compositions in sediment samples is presented. Separation of Cd and Pb was designed by using an anionic exchange chromatographic procedure. Measurements of Cd isotopic compositions were carried out by multi-collector inductively coupled plasma mass spectrometer (MC-ICPMS), by using standard-sample bracketing technology for mass bias correction and Pb isotopic ratios were determined by thermal ionization mass spectrometry (TIMS). The factors that affect the accurate and precise Cd isotope compositions analysis, such as instrumental mass fractionation and isobaric interferences, were carefully evaluated and corrected. The Cd isotopic results were reported relative to an internal Cd solution and expressed as the δ^114/110Cd. Five Cd reference solutions and one Pb standard were repeatedly measured in order to assess the accuracy of the measurements. Uncertainties obtained were estimated to be lesser than 0.11‰ (2s) for the δ^114/110Cd value. Analytical uncertainties in 2s for Pb isotopic ratios were better than 0.5‰. The method has been successfully applied to the investigation of Cd and Pb isotope compositions in sediment samples collected from North River in south China.     

Prompt k 0-factors and relative gamma-emission intensities for the strong non-1/v absorbers 113Cd, 149Sm, 151Eu and 155,157Gd

Prompt k ₀-factors relative to chlorine and relative g-emission intensities were determined for the strong non-1/v absorbers ¹¹³Cd, ¹⁴⁹Sm, ¹⁵¹Eu,¹⁵⁵Gd and ¹⁵⁷Gd. Measurements were performed using the SNU-KAERI prompt gamma activation analysis (PGAA) facility at the Korea Atomic Energy Research Institute (KAERI). For proper experimental determination of the prompt k ₀-factors, the effective g-factor and cadmium ratio were taken into account, in consideration of the effects from the non-1/v capture cross section and neutron spectrum in the thermal and epithermal energy region. By using the actual spectrum of the neutron beam in this study, the effective g-factor was obtained by calculation, and the influence of epithermal neutrons on the capture rate was corrected by measuring the cadmium ratio for each non-1/v target isotope. The measured prompt k ₀-factors were used to check the consistency between the existing dataset of the absolute g-emission intensity and the 2200 m/s capture cross section for these isotopes.     

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.     

Characterization of neutron transmuted zinc traces in pure copper materials by isotope dilution mass spectrometry

The neutron transmutation doping (NTD) of highly pure copper with zinc was investigated as a promising means of achieving controlled gradation of the zinc content in the range 1–20 μg g^–1. The doping process leads to the enrichment of two stable isotopes ⁶⁴Zn and ⁶⁶Zn in a ratio which differs from that of natural isotopic distribution. Mass spectrometric investigations by thermal ionization mass spectrometry (TIMS) were performed to validate the results obtained by gamma spectrometry. The investigations included both determination of the isotopic ratios of the doped zinc isotopes and the analysis of the accumulated zinc contents by isotope dilution (ID) analysis. Thereby a sample-specific correction of the blank could be performed because the isotope ⁶⁸Zn was not influenced, because of the transmutation process. The results obtained by TIMS prove the strict proportionality of the doped zinc content, in the range 5 to 20 μg g^–1, to the neutron fluence. Comparison with gamma spectrometric results showed a very good agreement within the uncertainties.     

Isotope shift studies in the spectra of Gadolinium in UV region and term shifts of high even levels of Gd I

Isotope shift Δσ(¹⁵⁶Gd?¹⁶⁰Gd) is reported in 70 spectral lines of neutral gadolinium atom (Gd I) in the 3290- 3920 Å region providing isotope shift data in UV lines of Gd I spectrum for the first time. The measurements were carried out on a photoelectric recording Fabry-Perot Spectrometer using highly enriched isotopic samples of gadolinium. Term isotope shifts ΔT(¹⁵⁶Gd?¹⁶⁰Gd) have been evaluated for 48 high lying even parity energy levels of Gd I using this data; new ΔT values have been obtained for 24 levels. Electronic configurations 4f⁷5d6s6p, 4ff⁷5df²6p and 4f⁸5d6s assigned earlier to these even levels have been either confirmed or configuration mixing pointed out in some of these levels. Probable assignment of 4f⁸5d6s configuration to 8 even levels between 32 930 and 35 500 cm^-1 have been confirmed.     

A quick method for the determination of the Al/Si weight ratio in alumino-silicates using an Am-Be neutron source

An irradiation procedure with fast and thermal neutrons from a 5 Ci Am-Be isotopic neutron source irradiation facility in combination with a 3'3' NaI(Tl) detector system has been used to determine Al/Si weight ratios in alumino-silicates. Samples were irradiated with and without Cd cover for 10 minutes and counted for 10 minutes after a waiting time of 1 minute. The peak area analysis of the 1779 keV gamma-ray line of ²⁸Al product radionuclide produced via ²⁷Al(n,γ)²⁸Al and ²⁸Si(n,p)²⁸Al reactions in combination with the neutron flux parameter at the irradiation site and nuclear data were used to determine Al/Si ratios. Due to discrepancy in literature data, Am-Be neutron source spectrum averaged cross sections of (n,p) reactions on ²⁷Al, ²⁸Si and ⁵⁶Fe were determined by the activation technique using ¹¹⁵In(n,n')^115mIn as the fast neutron flux monitor reaction. The method was tested using mixtures of high-purity Al₂O₃ and SiO₂ with known weight ratios of Al/Si and validated by a certified reference material BCS-CRM 348 (Ball Clay). Results are presented for bentonite, kaolin, bauxite, feldspar and ball clay samples from Nigeria. The method is non-destructive, rapid and suitable for use in-situ for large-scale exploration works and industrial process control. This revised version was published online in July 2006 with corrections to the Cover Date.     

A pre-concentration neutron activation analysis method for the determination of 232Th utilizing a dry-tube irradiation facility

A revized method for determining ²³²Th using a pre-concentration neutron activation analysis (PCNAA) procedure was developed to accommodate irradiation in a dry irradiation tube environment. ²³²Th extracted by ion-exchange from a sample was electrodeposited onto 5/8″ diameter vanadium planchets, which are arranged in a stack and irradiated in the dry tube central irradiation facility (CIF) of the reactor. The higher neutron fluence of this facility improved sensitivity by approximately 37%, however, the higher temperatures required modifications to the irradiation procedure. Because the heat in the CIF would melt the plastic spacers used in the original method, a tube of high-purity quartz was used to contain samples, and high purity quartz spacers were used to separate the vanadium planchets during the irradiation. Test irradiations have determined that no significant transfer occurred from the disks to the silica disks and no significant variation in the neutron flux was observed. Finally, a thin film barrier was tested for its ability to reduce recoil contamination from ²²⁹Th onto the detector during alpha spectroscopy. The film was shown to reduce contamination to levels indistinguishable from normal background.     

Measurements of the neutron spectra from the 7Li(p,n) accelerator based neutron source: Position and angular dependences

Thick target ⁷Li(p,n) neutron spectra were measured using a ³He ion chamber in the proton energy range of 1.95 to 2.30 MeV. The fast neutron spectra were collected for various distances from the lithium target as well as for various neutron emission angles. By unfolding the ³He raw data with the iterative van Cittert algorithm, the neutron fluence spectra were obtained. The ³He measured neutron spectra were compared with both analytically computed and Monte Carlo simulated spectra to account for neutron scatterings in the lithium target assembly and in the experimental area. To verify the accuracy of the neutron dose computation, the fast neutron kerma was obtained for each neutron spectrum using the fluence to kerma conversion coefficients and was compared with the measured neutron dose using tissue-equivalent proportional counters. In the position dependence investigation at the 0° emission angle, the analytically computed neutron kerma overestimates the experimental kerma by a factor of two mainly due to neutron moderation. The corresponding neutron kerma from the ³He measured spectra were in agreement with the neutron doses measured using tissue-equivalent proportional counters within 20% for lower proton energies, but the discrepancy increased to ～50% for higher proton energies. In the angular distribution investigation, a notable discrepancy between measured and computed neutron spectra were observed due to the neutron scattering effects in the target assembly and experimental room.     

Chemical process study on the separation of gadolinium-153

Three routes of chemical processes for a multicurie production of¹⁵³Gd have been established and demonstrated using one gram of Eu₂O₃ as target irradiated under a neutron flux of 5.0·10¹³n/cm²/s for 42 days. Simulated experiments with the synthetic solution containing appropriate amounts of Gd and Eu and the tracers were performed throughout the established chemical process for verifying its feasibility and the effectiveness. The results show that a high specific activity of 100 Ci/g Gd with the desired radionuclide purity of greater than 99.999% of¹⁵³Gd can be obtained. The chemical yield and processing time among the processes were compared.     

The determination of235U/238U ratios by activation analysis utilizing high resolution γ-spectrometry

The application of high resolution γ-spectrometry to the direct determination of²³⁵U/²³⁸U isotopic ratios in small uranium samples after neutron activation is reported. The consistency obtained relative to mass spectrometrically determined isotopic ratios is better than 5% for isotopic ratios between 0.06885 and 1.095. The method is not subject to the main disadvantages of the known radiochemical methods for²³⁵U/²³⁸U isotopic ratio determinations, and should be appreciably more rapid compared to the solid-source mass spectrometric method giving the same precision.     

High conduction neutron absorber to simulate fast reactor environment in an existing test reactor

A new metal matrix composite material has been developed to serve as a thermal neutron absorber for testing fast reactor fuels and materials in an existing pressurized water reactor. The performance of this material was evaluated by placing neutron fluence monitors within shrouded and unshrouded holders and irradiating for up to four cycles. The monitor wires were analyzed by gamma and X-ray spectrometry to determine the activities of the activation products. Adjusted neutron fluences were calculated and grouped into three bins—thermal, epithermal, and fast—to evaluate the spectral shift created by the new material. A comparison of shrouded and unshrouded fluence monitors shows a thermal fluence decrease of ~11 % for the shielded monitors. Radioisotope activity and mass for each of the major activation products is given to provide insight into the evolution of thermal absorption cross-section during irradiation. The thermal neutron absorption capability of the composite material appears to diminish at total neutron fluence levels of ~8 × 10²⁵ n/m². Calculated values for dpa in excess of 2.0 were obtained for two common structural materials (iron and nickel) of interest for future fast flux experiments.     

Isotope shift studies in the UV spectrum of singly ionised gadolinium

Isotope shift Δσ(¹⁵⁶Gd-¹⁶⁰Gd) are reported for 33 spectral lines of singly ionised gadolinium (Gd II) in the 3315–3930 Å region, making use of a photoelectric recording Fabry-Perot spectrometer and highly enriched isotopic samples of ¹⁵⁶Gd and ¹⁶⁰Gd Isotope shift values for these lines have not been reported earlier. Using this data, term isotope shift ΔT(¹⁵⁶Gd-¹⁶⁰Gd) have been evaluated for the even and odd parity energy levels involved in these transitions. We report here ΔT values of only 10 odd parity energy levels lying above 35 000 cm⁻¹, which have been evaluated for the first time. Configuration assignments of six of these levels to 4f⁸6p have been confirmed and probable configurations suggested for four unassigned levels.     

Determination of <Emphasis Type="Italic">k</Emphasis><Subscript>0</Subscript>-values for some elements in neutron capture gamma-ray for prompt gamma activation analysis

Exploration and modification of data for k ₀-PGAA (prompt γ-ray activation analysis) values used as standards for k ₀ standardization are needed. An integrated system has been installed and calibrated in Hot Laboratories Center for PGAA, using ²⁵²Cf isotopic neutron source with neutron flux of 6.16E8 n/cm² s. The prompt k ₀-factors of about 12 elements were determined versus the 1951.1 keV γ-ray of the ³⁵Cl, as well as analyzing crude oil and oil product samples. The concentrations of the elements in crude oil H, B, Mg, Al, Na, Si, P, S, Cl, V and Cd were 1.18E5, 0.084, 5.48E2, 8.45E2 4.88E2, 1.62E2, 3.72E2, 8.2, 144.3, 393 and 209.2 ppm while in oil product samples were 1.32E5, 5.87, 4.56E2, 4.22E2, 7.16E3, 699, 157, 8.74, 492.3, 61 and 198.2 ppm. Validation of the k ₀-PGAA was applied in analyzing standard IAEA reference material (soil-7) which give good agreement with the literature data. The ²⁵²Cf neutron beam in radiation position was characterized by the cadmium-ratio method, and found that the cadmium ratio (f), was 160.