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Atomic Energy of Canada Limited FISSION PRODUCT DATA FOR Atomic Energy of Canada Limited FISSION PRODUCT DATA FOR THERMAL REACTORS PART II - YIELDS by W.H. WALKER \ \ Chalk River Nuclear Laboratories V *- ( 1 Chalk Rivet, Ontario April 1973 ' AECL-3037 FISSION PRODUCT DATA FGR THERMAL REACTORS PART II - YIELDS by W. H. Walker Chalk River Nuclear Laboratories Chalk River, Ontario April 1973 AECL-3037 Part II FISSION PRODUCT DATA FOR THERMAL REACTORS PART II - YIELDS by W. H. Walker ABSTRACT Thermal neutron cumulative fission yields from 335u, 833U, 339Pu and 241Pu are reviewed. Particular attention is given to mass spectrometric data which accounts for the greater fraction of the total yields. A three-step treatment of spectrometric data is used: first, the concentrations of isotopes of each fission product element are determined to define the local shape of the yield vs. mass curve; second, the relative numbers of atoms of each element formed in fission are derived from isotope dilution or isobaric coupling measurements thus linking together all the isotopic concentrations of both the light or heavy mass peaks to obtain the shape over the entire mass spectrometric range; third, the mass spectrometric data are normalized using isotope dilution measurements of the number of fissions and radiometric and interpolated fields. In general, the greatest source of uncertainty in the mass spectrometric range is the second step and appears to arise from systematic differences between the methods used in different laboratories. Manuscript prepared November 1972 Chalk River Nuclear Laboratories Chalk River, Ontario April 1973 AECL-3037 Part II Données sur les produits de fission pour les réacteurs thermiques Partie II - Rendements par W.H. Walker Résumé Les rendements cumulatifs de fission des 235 233 2 neutrons thermiques de U, U, 239pu et ^lpu sont passés en revue. Une attention particulière est accordée aux données de spectrométrie de masse qui constituent la plus grande partie des rendements totaux. Un traitement en trois étapes des données spectrométriques est employé: premièrement, les concentrations des isotopes de chaque élément de produit de fission sont déterminées pour définir la forme locale de la courbe "rendement-masse"; deuxièmement, les nombres relatifs des atomes de chaque élément formé au cours de la fission sont calculés à partir de la dilution isotopique ou des mesures de couplage isobarique, reliant ainsi ensemble toutes les concentrations Isotopiques des pics des masses lourdes et légères, afin d'obtenir la forme pour l'intervalle complet de la spectrométrie de masse; troisièmement, les données spectrométriques de masse sont normalisées au moyen d'une mesure par dilution isotopique, du nombre de fissions et des rendements radiométriques et interpolés. En général, la plus grande source d'incer- titude dans l'intervalle de la spectrométrie de masse est la deuxième ét-ipe. Elle semble provenir de différences systématiques entre les méthodes employées dans les différents laboratoires. Manuscrit rédigé en novembre 1972 L'Energie Atomique du Canada, Limitée Laboratoires Nucléaires de Chalk River Chalk River, Ontario Avril 1973 AECL-3037 Partie II TABLE OF CONTENTS Page 1. INTRODUCTION 2. RELATIVE ISOTOPICC ABUNDANCES 3 2.1 Krypton and Rubidium 4 2.2 Strontium and Y ":rium 6 2.3 Zirconium 7 2.4 Molybdenum 8 2.5 Ruthenium 9 2.6 Xenon 10 2.7 Cesium and Barium 12 2.8 Cerium 14 2.9 Neodymium 16 2.10 Samarium and Europium 18 3. RELATIVE ELEMENT YIELDS 21 3.1 33BU 23 3.2 333U 26 3.3 339Pu 28 3.4 341Pu 30 4. ERROR ASSIGNMENTS 32 5. COMPLETING THE YIELD DISTRIBUTIONS 35 5.1 33BU Fission 36 5.2 J33U Fission 40 5.3 aa9Pu Fission 46 5.4 341Pu Fission 47 6. SUMMARY 5l 7. ACKNOWLEDGMENTS 54 8. REFERENCES 55 TABLES Page 1. Relative Yields of Krypton and Rubidium isotopes 5 2. Relative Yields of Strontium and Yttrium isotopes 6 3. Relative Yields of Zirconium Isotopes 7 4. Relative Yields of Molybdenum Isotopes 8 5. Relative Yields of Ruthenium Isotopes 9 6. Relative Yields of Xenon Isotopes 11 7. Relative Yields of Cesium and Barium isotopes 13 8. Relative Yields of Cerium Isotopes 15 9. Relative Yields of Neodymium Isotopes Isotopes 17 10. Relative Yields of Samarium and Europium isotopes 20 11. Relative Element Yields in 33Bu Thermal Neutron 24 Fission 12. Normalized Mass Spectrometric Yields in 23Bu Thermal 25 Neutron Fission 13. Relative Element Yields in S3Cu Thermal Neutron 26 Fission 14. Normalized Mass Spectrometric Yields in a33u Thermal 27 Neutron Fission 15. Relative Element Yields in 339Pu Thermal Neutron 28 Fission 16. Normalized Mass Spectrometric Yields in 339Pu Thermal 29 Neutron Fission 17. Relative Element Yields in S41Pu Thermal Neutron 30 Fission 18. Normalized Mass Spectrometric Yields in 241Pu Thermal 31 Neutron Fission 19. Error Assignments for the Heavy Mass peak 33 20. Error Assignments for the Light Mass Peak 34 21. Yields of Light Mass Fission Products from 3BU 38 22. Yields of Heavy Mass Fission Products from a35u 39 23. Yields of Light Mass Fission Products from a33U 42 24. Yields of Heavy Mass Fission Products from a33u 43 25. Yields of Light Mass Fission Products from 339Pu 44 26. Yields of Heavy Mass Fission Products from 239Pu 45 27. Yields of Light Mass Fission Products from 341Pu 48 28. Yields of Heavy Mass Fission Products from 841Pu 49 29. Summary of Recommended Yields - Light Masses 52 30. Summary of Recommended Yields - Heavy Masses 53 FIGURES 1. Cumulative Yields vs Mass 61 2. Cumulative Yields vs Displacement from A, the mean mass g2 FISSION PRODUCT DATA FOR THERMAL REACTORS PART II - YIELDS by W. H. Walker 1. INTRODUCTION Fission product yield measurements have played an important part in the study of fission since its discovery. The main interest initially was the general shape of the fission fragment distribution as a function of mass, and this evolved into detailed studies of the deviations from the smooth distribution (fine structure). Recent work has been directed to precise yield measurements of specific fission products for use in the accurate determination of fuel burnup. It is surprising that the main interest in fission yields has never been their effect on fission product absorp- tion. Most of the effort in this field has been directed to determining nuclide cross sections accurately, even though neutron absorption by most fission products is proportional to both yield and cross section, in the important case of a rapidly saturating nuclide such as 136Xe and 149Sm, neutron absorption at equilibrium concentration (saturation) is primarily dependent on the yield and nearly independent of its cross section. In this evaluation all corrections to measured data for p-decay c>.nd neutron capture are reviewed and recalculated where necessary to provide as firm a base as possible for a set of recommended yields for th3rmal neutron fission of 33Bu, 333U, 239Pu and 341Pu. An assessment of uncertainties in these yield values is also provided so that, in future, the accuracy of fission product absorption calculations can be estimated wibh greater confidence. 1.1. Outline of Evaluation Methods The earliest yield measurements were of radioactive fission products using counting techniques. These gave absolute yields with large uncertainties or relative yields normalized to some standard such as 67-h 99Mo. Later, mass spectrometers were used to determine relative yields of tne fission product isotopes of a particular element. The intro- duction of isotope dilution techniques enabled mass spectro- metrists to determine absolute yields directly and radio- chemists to improve the accuracy of their absolute yield determinations. - 2 - Both radiometric and mass spectre-metric yield measurements are subject to the usual chemistry difficulties, but the latter have the advantage from the evaluator's viewpoint of yiving the shape of a portion of the "yield vs mass" curve (i.e. the relative yields) to a high precision. This advantage cannot be easily exploited because mass spectrometric yields are always assigned a single error which has, as its dominant component, the un- certainty in the number of fissions. Since all mass spectrometric yields are obtained in three steps it is the purpose of this evaluation to obtain the best set of data appropriate to each step and to determine what un- certainty each step contributes to the final uncertainty. First the yield vs mass curve is determined for each fission product element by comparing all mass spectrometric measurements of concentrations of fission product isotopes of that element (the isotopic abundance) for the fissile nuclide of interest. These shapes are then linked together to obtain the main portion of the yield vs mass distribution. The linking is done using either isotope dilution measurements, which give the number of atoms of each element per fission, or measured isotopic abundances of two isobars, each relative to other isotopes of its own element and then completing the link using known p-decay half-lives, and irradiation and decay times. The first method is subject to errors in chemistry, and the second to errors in half-lives or elapsed time. For thermal neutron fission of a36u several mass spectro- meter measurements have been made for each of the elements near the peak of the light and heavy mass distributions. In this case it is quite probable that an incorrect yield in one measure- ment, such as might be caused by an unidentified contamination at one mass, can be detected because the isotopic abundance at that mass differs significantly from the average. The situation for a33U, a39Pu and a41Pu is less satisfactory because fewer measurements are available. Also, the mass range measured is usually the same as for a35U, for which many of the techniques were developed, and covers a smaller fraction of the yield for 333U, a39Pu and a41Pu. The light mass peak in a41Pu fission is most poorly covered, with less than half the total light mass peak measured mass spectrometrically compared to 88% for a3Bu.
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