The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known (n, g) and (n, f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.
The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known or in some cases not measured (n,?) and (n, f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 239Pu, 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.
The maintenance of strong scientific expertise is criticalto the U.S. nuclear attribution community. It is particularly importantto train students in actinide chemistry and physics. Neutroncross-section data are vital components to strategies for detectingexplosives and fissile materials, and these measurements requireexpertise in chemical separations, actinide target preparation, nuclearspectroscopy, and analytical chemistry. At the University of California, Berkeley and the Lawrence Berkeley National Laboratory we have trainedstudents in actinide chemistry for many years. LBNL is a leader innuclear data and has published the Table of Isotopes for over 60 years. Recently, LBNL led an international collaboration to measure thermalneutron capture radiative cross sections and prepared the EvaluatedGamma-ray Activation File (EGAF) in collaboration with the IAEA. Thisfile of 35,000 prompt and delayed gamma ray cross-sections for allelements from Z=1-92 is essential for the neutron interrogation ofnuclear materials. LBNL has also developed new, high flux neutrongenerators and recently opened a 1010 n/s D+D neutron generatorexperimental facility.
The Surrogate nuclear reactions method, an indirect approach for determining cross sections for compound-nuclear reactions involving difficult-to-measure targets, is reviewed. Focusing on cross sections for neutron-induced reactions on actinides, we review the successes of past and present applications of the method and assess its uncertainties and limitations. The approximations used in the analyses of most experiments work reasonably well for (n, f) cross sections for neutron energies above 1-2 MeV, but lead to discrepancies for low-energy (n, f) reactions, as well as for (n, [gamma]) applications. Correcting for some of the effects neglected in the approximate analyses leads to improved (n, f) results. We outline steps that will further improve the accuracy and reliability of the Surrogate method and extend its applicability to reactions that cannot be approached with the present implementation of the method.
Directly measuring (n,2n) cross sections on short-lived actinides presents a number of experimental challenges: scattered beam can produce neutron backgrounds in the detectors, fission can produce a substantial neutron background, and created a target with a short-lived isotope can be extremely difficult. To perform these surrogate (n,2n) cross section measurements, a silicon telescope array has been placed along a beam line at the Texas A & M University Cyclotron Institute, which is surrounded by a large tank of Gadolinium-doped liquid scintillator, which acts as a neutron detector. The combination of the charge-particle and neutron-detector arrays is referred to as NeutronSTARS. In the analysis procedure for calculating the (n,2n) cross section, the neutron detection efficiency and time structure plays an important role. Due to the lack of availability of isotropic, mono-energetic neutron sources, modeling is an important component in establishing this efficiency and time structure. This report describes the NeutronSTARS array, which was designed and commissioned during this project. It also describes the surrogate reaction technique, specifically referencing a 235U(n,2n) commissioning measurement that was fielded during the past year.
The overall objective of this project is the measurement of neutron capture cross sections of importance to stewardship science and astrophysical modeling of nucleosynthesis, while at the same time helping to train the next generation of scientists with expertise relevant to U.S. national nuclear security missions and to stewardship science. A primary objective of this project is to study neutron capture cross sections for various stable and unstable isotopes that will contribute to the Science Based Stockpile Stewardship (SBSS) program by providing improved data for modeling and interpretation of nuclear device performance. Much of the information obtained will also be important in astrophysical modeling of nucleosynthesis. Measurements of these neutron capture cross sections are being conducted in collaboration with researchers at the Los Alamos Neutron Science Center (LANSCE) facility using the unique Detector for Advanced Neutron Capture Experiments (DANCE). In our early discussions with the DANCE group, decisions were made on the first cross sections to be measured and how our expertise in target preparation, radiochemical separations chemistry, and data analysis could best be applied. The initial emphasis of the project was on preparing suitable targets of both natural and separated stable europium isotopes in preparation for the ultimate goal of preparing a sufficiently large target of radioactive 155Eu (t1/2 = 4.7 years) and other radioactive and stable species for neutron cross-section measurements at DANCE. Our Annual Report, ''Neutron Capture Experiments on Unstable Nuclei'' by J.M. Schwantes, R. Sudowe, C.M. Folden III, H. Nitsche, and D.C. Hoffman, submitted to NNSA in December 2003, gives details about the initial considerations and scope of the project. During the current reporting period, electroplated targets of natural Eu together with valuable, stable, and isotopically pure 151Eu and 153Eu, and isotopically separated 154Sm were measured for the first time at the DANCE facility in early 2004. The Eu targets, suitable blanks, Be backing foils, and standards had been sent to the DANCE group in early fall 2003. Some preliminary data analysis was performed and more sophisticated analysis has begun. We developed plans for a suitable computer system for data analysis within our group at Berkeley and had meetings with counterparts at Lawrence Livermore National Laboratory (LLNL) and LANL concerning analysis of these data. Our major emphasis in 2004 has been to develop the separations and processes ultimately required to prepare radioactive targets of 4.7-year 155Eu. Efforts continued to devise an optimum multiprocess procedure suitable for use in separating radioactive 155Eu already produced by irradiation of stable 154Sm in a high neutron flux reactor at the Institut Laue-Langevin in France and shipped to LANL (the 22-min 155Sm neutron-capture product decays to 155Eu). This separation is extremely demanding because the highly radioactive 155Eu must be isolated from about 20 times as much mass of samarium before a target can be prepared for DANCE measurements. After all the procedures have been fully tested the radioactive 155Eu will be separated. The same electroplating methods already used successfully to prepare stable Eu isotope targets will be used to prepare the 155Eu target for DANCE. Discussions were held with LANL radiochemists in the Chemistry (C) Division about appropriate facilities at LANL for conducting the full-scale separation and purification of the radioactive targets. Three more multiprocess separations were developed that generated less chemical and radioactive waste, but they must still be adapted for processing hundred-milligram quantities. Until these separations can be successfully implemented at this scale, standard HPLC procedures will be used for separating and preparing radioactive 155Eu, 2.6-year 147Pm, and 1.9-year 171Tm target materials. Future directions beyond the preparation of radioactive lanthanide targets include closer collaboration with both LLNL and LANL to prepare actinide targets such as plutonium, americium, and curium. Also, the applicability of established and novel techniques will be evaluated for rapid separations of Am and Cm required in the irradiation of 241Am. Lastly, we will conduct a series of experiments aimed at enhancing current methods used to electrodeposit lanthanide and actinide targets on thin Ti and Be backings.
Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications in a wide energy range from sub-thermal energies up to 200 MeV. A parallel-plate ionization chamber are used to measure fission cross sections ratios relative to the 235U standard while incident neutron energies are determined using the time-of-flight method. Recent measurements include the {sup 233,238}U, 239−242Pu and 243Am neutron-induced fission cross sections. Obtained data are presented in comparison with ex isting evaluations and previous data.
This is an authoritative compilation of information regarding methods and data used in all phases of nuclear engineering. Addressing nuclear engineers and scientists at all levels, this book provides a condensed reference on nuclear engineering since 1958.
Experimentally determined neutron cross section data for heavy actinides involved in the reactor production chains leading to /sup 238/Pu and /sup 252/Cf were examined. The neutron energy region below one kilovolt is emphasized because these cross sections and reactions are important for thermal and near- thermal reactors. Included with the data summaries are brief descriptions of pertinent measurements in progress or plarmed for the near future at United States and European laboratories. Additional measurements that are needed are suggested. Of most immediate interest are: sigma /sub ny/ for /sup 248/Cm below 1 keV, sigma /sub nf/ for /sup 245/Cm below 40 eV, sigma /sub nf/ for /sup 247/ Cm below 40 eV, and sigma /sub nf/ for /sup 251/Cf below 1 keV. Data were gathered for the survey through January 1973. (auth).
