[en] This report documents the FY13 efforts to enhance a dataset of spent nuclear fuel isotopic composition data for use in developing intrinsic signatures for nuclear forensics. A review and collection of data from the open literature was performed in FY10. In FY11, the Spent Fuel COMPOsition (SFCOMPO) excel-based dataset for nuclear forensics (NF), SFCOMPO/NF was established and measured data for graphite production reactors, Boiling Water Reactors (BWRs) and Pressurized Water Reactors (PWRs) were added to the dataset and expanded to include a consistent set of data simulated by calculations. A test was performed to determine whether the SFCOMPO/NF dataset will be useful for the analysis and identification of reactor types from isotopic ratios observed in interdicted samples

[en] Scanning cargo transported via aircraft ('air cargo') for explosive threats is a problem that, at present, lacks a comprehensive technical solution. While explosives detection in the baggage-scanning domain has a rich history that sheds light on potential solutions for air cargo, baggage scanning differs in several ways and thus one cannot look to the present array of technologies. Some contemporary solutions, like trace analysis, are not readily applied to cargo due to sampling challenges while the larger geometry of air cargo makes others less effective. This review article examines an array of interrogation techniques using photons and neutrons as incident particles. We first present a summary of the signatures and observables explosives provide and review how they have been exploited in baggage scanning. Following this is a description of the challenges posed by the air cargo application space. After considering interrogation sources, methods focused on transmission imaging, sub-surface examination and elemental characterization are described. It is our goal to shed light on the technical promise of each method while largely deferring questions that revolve around footprint, safety and conduct of operations. Our overarching intent is that a comprehensive understanding of potential techniques will foster development of a comprehensive solution

[en] One of the fundamental activities within the field of nuclear forensics is the laboratory analysis of nuclear material; one aspect is providing the isotopic composition of the material under investigation. For both plutonium and uranium, this includes a unique suite of isotopes that, individually and collectively (i.e. an isotopic vector), will help characterize these materials, and potentially provide insight into their mode of production, intended utilization, and processing history. A full understanding of how this information is used provides the basis for defining the need for these measurements and helps determine the precision and accuracy requirements for those measurements. This paper provides an overview of this process as it applies to plutonium, discussing how reactor design and operating parameters can impact the resultant plutonium vector, thereby giving us the ability to infer those reactor traits based on isotopic measurements.

[en] This paper summarizes the results of an extension to an earlier study that examined the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with the PUREX, UREX+, and COEX reprocessing schemes. This study focuses on the materials associated with the UREX, COEX, THOREX, and PYROX reprocessing schemes. This study also examines what is required to render plutonium as 'unattractive.' Furthermore, combining the results of this study with those from the earlier study permits a comparison of the uranium and thorium based fuel cycles on the basis of the attractiveness of the SNM associated with each fuel cycle. Both studies were performed at the request of the United States Department of Energy (DOE), and are based on the calculation of 'attractiveness levels' that has been couched in terms chosen for consistency with those normally used for nuclear materials in DOE nuclear facilities. The methodology and key findings will be presented. Additionally, how these attractiveness levels relate to proliferation resistance (e.g. by increasing impediments to the diversion, theft, undeclared production of SNM for the purpose of acquiring a nuclear weapon), and how they could be used to help inform policy makers, will be discussed.

[en] Highlights: ► Common sources of error in transmission NEXAFS spectra in a STXM identified and shown to be significant. ► Three facile methods to characterize and eliminate or limit errors are detailed. ► Appropriate spectra processing methods are discussed and demonstrated. ► Quantitative compositional analysis of organic thin films is conducted and shown to be robust. -- Abstract: Near edge X-ray absorption fine structure (NEXAFS) spectroscopy is well suited for the quantitative determination of the composition of soft matter thin films. Combined with the high spatial resolution of a scanning transmission X-ray microscope, compositional maps of submicron morphologies can be derived and have been used successfully to characterize a number of materials systems. However, multiple sources of known systematic errors limit the accuracy and are frequently not taken into account. We show that these errors can be significant (more than 10%) and demonstrate simple methods to eliminate them. With suitable precautions, a compositional measurement can be made on a thin film sample in a matter of minutes with sub-micron spatial resolution and sub-percent compositional precision. NEXAFS measurements are furthermore known to be sensitive to anisotropic molecular orientation and a strategy to account for that and extract preferential molecular orientation relative to a reference is presented. The spatial resolution of the measurement can be increased to below 100 nm at the expense of compositional precision, depending on the point spread function of the zone plate focusing optics of the microscope.

[en] This paper is an extension to earlier studies that examined the attractiveness of materials mixtures containing special nuclear materials (SNM) and alternate nuclear materials (ANM) associated with the PUREX, UREX, COEX, THOREX, and PYROX reprocessing schemes. This study extends the figure of merit (FOM) for evaluating attractiveness to cover a broad range of proliferant state and sub-national group capabilities. The primary conclusion of this study is that all fissile material needs to be rigorously safeguarded to detect diversion by a state and provided the highest levels of physical protection to prevent theft by sub-national groups; no 'silver bullet' has been found that will permit the relaxation of current international safeguards or national physical security protection levels. This series of studies has been performed at the request of the United States Department of Energy (DOE) and is based on the calculation of 'attractiveness levels' that are expressed in terms consistent with, but normally reserved for nuclear materials in DOE nuclear facilities. The expanded methodology and updated findings are presented. Additionally, how these attractiveness levels relate to proliferation resistance and physical security are discussed.

[en] We must anticipate that the day is approaching when details of nuclear weapons design and fabrication will become common knowledge. On that day we must be particularly certain that all special nuclear materials (SNM) are adequately accounted for and protected and that we have a clear understanding of the utility of nuclear materials to potential adversaries. To this end, this paper examines the attractiveness of materials mixtures containing SNM and alternate nuclear materials associated with the plutonium-uranium reduction extraction (Purex), uranium extraction (UREX), coextraction (COEX), thorium extraction (THOREX), and PYROX (an electrochemical refining method) reprocessing schemes. This paper provides a set of figures of merit for evaluating material attractiveness that covers a broad range of proliferant state and subnational group capabilities. The primary conclusion of this paper is that all fissile material must be rigorously safeguarded to detect diversion by a state and must be provided the highest levels of physical protection to prevent theft by subnational groups; no 'silver bullet' fuel cycle has been found that will permit the relaxation of current international safeguards or national physical security protection levels. The work reported herein has been performed at the request of the U.S. Department of Energy (DOE) and is based on the calculation of 'attractiveness levels' that are expressed in terms consistent with, but normally reserved for, the nuclear materials in DOE nuclear facilities. The methodology and findings are presented. Additionally, how these attractiveness levels relate to proliferation resistance and physical security is discussed.

[en] This paper examines the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with the various processing steps required for a closed fuel cycle. This paper combines the results from earlier studies that examined the attractiveness of SNM associated with the processing of spent light water reactor (LWR) fuel by various reprocessing schemes and the recycle of plutonium as a mixed oxide (MOX) fuel in LWR with new results for the final, repeated burning of SNM in fast-spectrum reactors: fast reactors and accelerator driven systems (ADS). The results of this paper suggest that all reprocessing products evaluated so far need to be rigorously safeguarded and provided moderate to high levels of physical protection. These studies were performed at the request of the United States Department of Energy (DOE), and are based on the calculation of 'attractiveness levels' that has been couched in terms chosen for consistency with those normally used for nuclear materials in DOE nuclear facilities. The methodology and key findings will be presented. Additionally, how these attractiveness levels relate to proliferation resistance (e.g. by increasing impediments to the diversion, theft, or undeclared production of SNM for the purpose of acquiring a nuclear weapon), and how they could be used to help inform policy makers, will be discussed.

[en] We report high-resolution X-ray diffraction studies of combinatorial epitaxial Ge (0 0 1) thin-films with varying doping concentrations of Co and Mn grown on Ge (0 0 1) substrates. The crystalline structure of the epitaxial thin-film has been determined using crystal-truncation rod (CTR) measurements and fitting analysis. By analyzing the fine interference fringes in the CTR intensity profile, strain sensitivity of ∼0.003% has been achieved. Using this method, the evolution of interfacial structures has been quantified as a function of doping concentration

[en] Scanning cargo transported via aircraft ('air cargo') for explosive threats is a problem that presently lacks a comprehensive technical solution. While chemical explosives detection in the baggage-scanning domain has a rich history that sheds light on potential solutions, air cargo differs in several important ways, and thus one cannot look to the present array of technologies. Some contemporary solutions, such as trace analysis, are not readily applied to cargo because of sampling challenges while the larger geometry of air cargo makes others less effective. This review article examines an array of interrogation techniques using photons and neutrons as incident particles. We first present a summary of the signatures and observables chemical explosives provide and review how they have been exploited in baggage scanning. Following this review is a description of the challenges posed by the air-cargo application space. After considering sources of photons and neutrons, we describe methods focused on transmission imaging, sub-surface examination, and elemental characterization. It is our goal to expand the understanding of each method's technical promise while largely deferring questions that revolve around footprint, safety, and conduct of operations. Our overarching intent is that a comprehensive understanding of potential techniques will foster the development of a comprehensive solution.