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Nuclear Data Sheets for A = 133

Evaluated nuclear structure and decay data for all nuclei within the A=133 mass chain are presented. The experimental data are evaluated and best values for level and gamma-ray energies, quantum numbers, lifetimes, gamma-ray intensities, and other nuclear properties are recommended. Inconsistencies and discrepancies that exist in the literature are noted. This work supersedes the earlier evaluation by S. Raab (1995Ra12), published in Nuclear Data Sheets75, 491 (1995).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Further Development of an ISOCS - based Advanced In Situ Gamma Spectrometry Services Tool for Waste Measurements - 17452

Canberra's In Situ Object Counting System is an established tool used for gamma spectrometry allowing a physical representation of complex geometries and mathematical calculation of the calibration function while avoiding the need for radioisotope standards. The ISOCS Uncertainty Estimator tool can be used to calculate defensible systematic calibration uncertainties. However the uncertainties depend on knowledge of the properties of the item being measured and for poorly characterized materials these can be large, often leading to large costs for waste sentencing. An ISOCS-based advanced in-situ gamma spectrometry services tool has been developed to reduce those uncertainties. This system is based on generating and comparing a range of candidate geometry models that yield figures of merit indicative of improved consistency between modelled data and available diverse measurement data. The approach and results of initial performance testing have previously been published, demonstrating an analysis procedure and enhanced accuracy for measurement of a low density 200 litre waste drum, based on measurements with known sources placed at different positions. It was shown how the accuracy of assay of Am-241 in a light matrix can be significantly improved. Further analysis has now been performed, with reference to measurements of a second drum, containing a standard matrix of higher density, and with a multiple radionuclide line source (Ba-133, Cs-137, Eu-152 and Am-241). These measurements represent a more challenging waste assay scenario, corresponding to potentially much larger assay uncertainties. Our results show how the assay uncertainty can be reduced, by careful application of AIGS, from relative values of the order of 100% to a few 10's of %. Furthermore, we demonstrate, through extended analysis of the test drum data, how an AIGS measurement program can be optimized to reduce the number of required measurement positions substantially. This paper describes these new results with comment on their importance and potential application for real waste assay projects. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of beta-decay rates for Ag 108, Ba 133, Eu 152, Eu 154, Kr 85, Ra 226, and Sr 90, measured at the Physikalisch-Technische Bundesanstalt from 1990 to 1996

We present the results of an analysis of measurements of the beta-decay rates of Ag 108, Ba 133, Eu 152, Eu 154, Kr 85, Ra 226, and Sr 90 acquired at the Physikalisch-Technische Bundesanstalt from 1990 through 1995. Although the decay rates vary over a range of 165 to 1 and the measured detector current varies over a range of 19 to 1, the detrended and normalized count rate measurements exhibit a sinusoidal annual variation with amplitude in the small range 0.068%-0.088% (mean 0.081%, standard deviation 0.0072%, a rejection of the zero-amplitude hypothesis) and phase-of-maximum in the small range 0.062-0.083 (January 23 to January 30). In comparing these results with those of other related experiments that yield different results, it may be significant that this experiment, at a standards laboratory, seems to be unique in using a 4π detector. These results are compatible with a solar influence, and do not appear to be compatible with an experimental or environmental influence. It is possible that Ba 133 measurements are also subject to a non-solar (possibly cosmic) influence.

79 ASTRONOMY AND ASTROPHYSICS↗

Low background HPGe spectrometer in investigations of 2β decay

The low background high sensitive HPGe spectrometer called OBELIX is briefly described. The calibration measurements using {sup 152}Eu, {sup 133}Ba and La{sub 2}O{sub 3} sources in different geometries, the obtained efficiency curves for OBELIX HPGe detector, the results of measurements of radioactivity of the NEMO-3 sources ({sup 100}Mo, {sup 150}Nd) as well as future plans for OBELIX detector (e.g. 0νEC/EC decay of {sup 106}Cd) are presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Design and testing of a combined neutron and gamma assay system for measuring fissile material in fuel and waste items - 15340

A combined neutron and gamma ray assay system for the measurement of fissile material in both fuel and waste items has been designed, modelled, developed and tested. The purpose of the system is to measure and characterize a wide range of fissile materials including uranium, plutonium, americium and mixed oxide fuel arising from a variety of processes and facilities across the United Kingdom. Dounreay Site Restoration Limited at Dounreay currently stores these items form the United Kingdom Nuclear Decommissioning Authority's un-irradiated fuel inventory. This inventory comprises historic materials from ex-United Kingdom Atomic Energy Authority nuclear fuel projects and experiments together with fast reactor fuel materials and some commercial fuel items as delivered to Dounreay for recovery. The combined assay system has been designed and constructed to support the operation of a fuel processing facility, which will be operated at Dounreay to treat these historic legacy fuel materials, making them suitable for long term storage. Appropriate characterization of the fissile material is required for safety, criticality control and nuclear materials safeguards purposes prior to final disposition. The system consists of both gamma ray and neutron measurement components. The results of a neutron measurement are combined with the gamma ray isotopic ratio measurement results to generate the assay result for the fissile material being characterized. The gamma ray component of the system employs a safeguards quality high purity Germanium detector with electro-mechanical cooling and the measurements of fissile material containers are made in a shielded chamber with a tin and copper graded lining. Containers of fissile material are rotated during the gamma ray measurement and a variable automatic steel collimator aperture mechanism is employed to adjust the measured count rate to control detector dead time. Gamma ray spectra are analysed using the plutonium and uranium isotopic ratio code PC/FRAM. The gamma ray system can also be configured to perform a direct assay of small quantities of uranium bearing material. For this assay measurement a series of cadmium filters can be positioned in front of the detector to reduce the contribution from 59 keV gamma rays from Am-241. In addition to gamma ray isotopic measurements, both active and passive neutron assay is performed by the system. The neutron-measuring component consists of a thick walled cylindrical polyethylene chamber, which provides neutron moderation for 30 one-inch diameter He-3 detector tubes located in re-entrant channels in the polyethylene moderator. Two removable polyethylene-inserts incorporating lower plug assemblies are provided, one with and one without a cadmium lining. Also two top plug units are provided, again one with cadmium and one without a cadmium liner. The Neutron Subsystem can be operated both as a passive and as an active neutron coincidence counter. In both fast and thermal active neutron mode, the neutron component employs two americium-beryllium (Am-Be) alpha-n neutron sources, one positioned in the top and the other in the bottom plug unit. The neutron sources are removed when the counter is operated in passive mode. Passive neutron detection efficiency and active neutron performance has been modelled using the MCNP Monte Carlo computer simulation code as part of the design process. In the absence of fissile samples, operation of the gamma ray component of the system has been tested initially using calibrated Eu-152 and Ba-133 gamma ray sources and the use of archived spectra from fissile material measurements. Initial testing of the neutron system has employed a calibrated Cf-252 spontaneous fission neutron source. Neutron testing has been confirmed using further MCNP simulations. The results of test measurements with the system are presented and compared with the results of MCNP measurement simulations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

New approach for calibration the efficiency of HpGe detectors

This work evaluates the efficiency calibrating of HpGe detector coupled with Canberra GC3018 with Genie 2000 software and Ortec GEM25-76-XLB-C with Gamma Vision software; available at Neutron activation analysis laboratory in Malaysian Nuclear Agency (NM). The efficiency calibration curve was constructed from measurement of an IAEA, standard gamma–point sources set composed by {sup 214}Am, {sup 57}Co, {sup 133}Ba, {sup 152}Eu, {sup 137}Cs and {sup 60}Co. The efficiency calibrations were performed for three different geometries: 5, 10 and 15 cm distances from the end cap detector. The polynomial parameters functions were simulated through a computer program, MATLAB in order to find an accurate fit to the experimental data points. The efficiency equation was established from the known fitted parameters which allow for the efficiency evaluation at particular energy of interest. The study shows that significant deviations in the efficiency, depending on the source-detector distance and photon energy.

42 ENGINEERING↗

Instrument for precision long-term β-decay rate measurements

We describe an experimental setup for making precision measurements of relative β-decay rates of {sup 22}Na, {sup 36}Cl, {sup 54}Mn, {sup 60}Co, {sup 90}Sr, {sup 133}Ba, {sup 137}Cs, {sup 152}Eu, and {sup 154}Eu. The radioactive samples are mounted in two automated sample changers that sequentially position the samples with high spatial precision in front of sets of detectors. The set of detectors for one sample changer consists of four Geiger-Müller (GM) tubes and the other set of detectors consists of two NaI scintillators. The statistical uncertainty in the count rate is few times 0.01% per day for the GM detectors and about 0.01% per hour on the NaI detectors. The sample changers, detectors, and associated electronics are housed in a sealed chamber held at constant absolute pressure, humidity, and temperature to isolate the experiment from environmental variations. The apparatus is designed to accumulate statistics over many years in a regulated environment to test recent claims of small annual variations in the decay rates. We demonstrate that absent this environmental regulation, uncontrolled natural atmospheric pressure variations at our location would imprint an annual signal of 0.1% on the Geiger-Müller count rate. However, neither natural pressure variations nor plausible indoor room temperature variations cause a discernible influence on our NaI scintillator detector count rate.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Reactor Fuel Isotopics and Code Validation for Nuclear Applications

Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133 Cs and 153 Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied as much as 10% of the measured values, and 109 Ag was consistently over-predicted by as much as 170%. In general, there is a larger uncertainty for modeling radioactive fission products when compared to either the actinides or the stable fission products in SNF. The relative C/E ratios ranged from a few percent for 137 Cs up to 60% and 100% for 106 Ru and 125 Sb, respectively. Limited or no radioactive fission products data exist in the current data sets for reactor types other than PWRs and BWRs. More work is needed in obtaining a greater diversity of radioactive fission product data. While performing this survey, issues leading to inconsistencies in nuclear fission yield data were discovered that specifically impacted the fission product noble gases. Emphasis was given to this legacy data, and corrective actions were taken as described in this report. After the fission yield data were corrected, the stable xenon and krypton fission products were predicted to within 5% of their measurements. However, preliminary results not explicitly given in this report indicate that the relative C/E ratio for the radioactive isotope 85 Kr varied as much as 10%. Due to the complex migration and the difficulty in measuring noble gases in the fuel, a more thorough investigation is needed to understand how accurately depletion codes can calculate these gas concentrations.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗