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Study of Chemical Changes in Uranium Oxyfluoride Particles Progress Report March - October 2009

Description: Nuclear forensics relies on the analysis of certain sample characteristics to determine the origin and history of a nuclear material. In the specific case of uranium enrichment facilities, it is the release of trace amounts of uranium hexafluoride (UF{sub 6}) gas - used for the enrichment of uranium - that leaves a process-characteristic fingerprint. When UF{sub 6} gas interacts with atmospheric moisture, uranium oxyfluoride particles or particle agglomerates are formed with sizes ranging from several microns down to a few tens of nanometers. These particles are routinely collected by safeguards organizations, such as the International Atomic Energy Agency (IAEA), allowing them to verify whether a facility is compliant with its declarations. Spectrometric analysis of uranium particles from UF{sub 6} hydrolysis has revealed the presence of both particles that contain fluorine, and particles that do not. It is therefore assumed that uranium oxyfluoride is unstable, and decomposes to form uranium oxide. Understanding the rate of fluorine loss in uranium oxyfluoride particles, and the parameters that control it, may therefore contribute to placing boundaries on the particle's exposure time in the environment. Expressly for the purpose of this study, we prepared a set of uranium oxyfluoride particles at the Institute for Reference Materials and Measurements (EU-JRC-IRMM) from a static release of UF{sub 6} in a humid atmosphere. The majority of the samples was stored in controlled temperature, humidity and lighting conditions. Single particles were characterized by a suite of micro-analytical techniques, including NanoSIMS, micro-Raman spectrometry (MRS), scanning (SEM) and transmission (TEM) electron microscopy, energy-dispersive X-ray spectrometry (EDX) and focused ion beam (FIB). The small particle size was found to be the main analytical challenge. The relative amount of fluorine, as well as the particle chemical composition and morphology were determined at different stages in the ageing process, and immediately after preparation. This ...
Date: November 22, 2009
Creator: Kips, R; Kristo, M & Hutcheon, I
Partner: UNT Libraries Government Documents Department

Geolocation and route attribution in illicit trafficking of nuclear materials

Description: We present a matrix of 60 possible forensic tools. If the specifics of the types of materials and analytical techniques are included, the number becomes vastly greater. Accordingly, the prioritization and discretion is addressed that should be utilized to select the most useful tools.
Date: April 1, 1999
Creator: Hutcheon, I & Niemeyer, S
Partner: UNT Libraries Government Documents Department

Action Sheet 36 Final Report

Description: Pursuant to the Arrangement between the European Commission DG Joint Research Centre (EC-JRC) and the Department of Energy (DOE) to continue cooperation on research, development, testing, and evaluation of technology, equipment, and procedures in order to improve nuclear material control, accountancy, verification, physical protection, and advanced containment and surveillance technologies for international safeguards, dated 1 September 2008, the IRMM and LLNL established cooperation in a program on the Study of Chemical Changes in Uranium Oxyfluoride Particles under IRMM-LLNL Action Sheet 36. The work under this action sheet had 2 objectives: (1) Achieve a better understanding of the loss of fluorine in UO{sub 2}F{sub 2} particles after exposure to certain environmental conditions; and (2) Provide feedback to the EC-JRC on sample reproducibility and characteristics.
Date: February 24, 2012
Creator: Kips, R. E.; Kristo, M. J. & Hutcheon, I. D.
Partner: UNT Libraries Government Documents Department

Analysis of bacterial spore permeability to water and ions using Nano-Secondary Ion Mass Spectrometry (NanoSIMS)

Description: Regulation of bacterial spore solvent and solute permeability is a fundamental feature of dormancy but is poorly understood. Here we present a new technique, nano-scale secondary ion mass spectrometry (NanoSIMS) that allows the direct visualization and quantification of chemical gradients within spores. Using NanoSIMS, we demonstrate the penetration of water and a simple ionic salt, LiF, into the core of Bacillus thuringiensis israelensis (Bti) spores. The results demonstrate chemical gradients spanning the outer coat to the inner spore core that are driven by concentration-dependent ionic fluxes. Using deuterated water (D{sub 2}O), we have shown that external water is either retained or exchanged with water contained within the spore. Hydration and exchange are rapid, on a timescale of < 1 minute. Our results suggest a permeation mechanism by which short-time scale diffusion into and out of the spore can occur along hydration pathways. Additional studies are in progress to define the flux rates and mechanisms controlling these processes.
Date: November 17, 2005
Creator: Ghosal, S; Fallon, S; Leighton, T; Wheeler, K; Hutcheon, I & Weber, P K
Partner: UNT Libraries Government Documents Department

Nuclear Forensics and Attribution for Improved Energy Security: The Use of Taggants in Nuclear Fuel

Description: The Global Nuclear Energy Partnership (GNEP), recently announced by DOE Secretary Bodman, poses significant new challenges with regard to securing, safeguarding, monitoring and tracking nuclear materials. In order to reduce the risk of nuclear proliferation, new technologies must be developed to reduce the risk that nuclear material can be diverted from its intended use. Regardless of the specific nature of the fuel cycle, nuclear forensics and attribution will play key roles to ensure the effectiveness of nonproliferation controls and to deter the likelihood of illicit activities. As the leader of the DHS nuclear and radiological pre-detonation attribution program, LLNL is uniquely positioned to play a national leadership role in this effort. Ensuring that individuals or organizations engaged in illicit trafficking are rapidly identified and apprehended following theft or diversion of nuclear material provides a strong deterrent against unlawful activities. Key to establishing this deterrent is developing the ability to rapidly and accurately determine the identity, source and prior use history of any interdicted nuclear material. Taggants offer one potentially effective means for positively identifying lost or stolen nuclear fuels. Taggants are materials that can be encoded with a unique signature and introduced into nuclear fuel during fuel fabrication. During a nuclear forensics investigation, the taggant signature can be recovered and the nuclear material identified through comparison with information stored in an appropriate database. Unlike serial numbers or barcodes, microtaggants can provide positive identification with only partial recovery, providing extreme resistance to any attempt to delete or alter them.
Date: April 5, 2007
Creator: Kristo, M J; Robel, M & Hutcheon, I D
Partner: UNT Libraries Government Documents Department

Chemical imaging of biological materials by NanoSIMS using isotopic and elemental labels

Description: The NanoSIMS 50 combines unprecedented spatial resolution (as good as 50 nm) with ultra-high sensitivity (minimum detection limit of {approx}200 atoms). The NanoSIMS 50 incorporates an array of detectors, enabling simultaneous collection of 5 species originating from the same sputtered volume of a sample. The primary ion beam (Cs{sup +} or O{sup -}) can be scanned across the sample to produce quantitative secondary ion images. This capability for multiple isotope imaging with high spatial resolution provides a novel new approach to the study of biological materials. Studies can be made of sub-regions of tissues, mammalian cells, and bacteria. Major, minor and trace element distributions can be mapped on a submicron scale, growth and metabolism can be tracked using stable isotope labels, and biogenic origin can be determined based on composition. We have applied this technique extensively to mammalian and prokaryotic cells and bacterial spores. The NanoSIMS technology enables the researcher to interrogate the fate of molecules of interest within cells and organs through elemental and isotopic labeling. Biological applications at LLNL will be discussed.
Date: April 10, 2006
Creator: Weber, P K; Fallon, S J; Pett-Ridge, J; Ghosal, S & Hutcheon, I D
Partner: UNT Libraries Government Documents Department

Bioforensics: Characterization of biological weapons agents by NanoSIMS

Description: The anthrax attacks of Fall 2001 highlight the need to develop forensic methods based on multiple identifiers to determine the origin of biological weapons agents. Genetic typing methods (i.e., DNA and RNA-based) provide one attribution technology, but genetic information alone is not usually sufficient to determine the provenance of the material. Non-genetic identifiers, including elemental and isotopic signatures, provide complementary information that can be used to identify the means, geographic location and date of production. Under LDRD funding, we have successfully developed the techniques necessary to perform bioforensic characterization with the NanoSIMS at the individual spore level. We have developed methods for elemental and isotopic characterization at the single spore scale. We have developed methods for analyzing spore sections to map elemental abundance within spores. We have developed rapid focused ion beam (FIB) sectioning techniques for spores to preserve elemental and structural integrity. And we have developed a high-resolution depth profiling method to characterize the elemental distribution in individual spores without sectioning. We used these newly developed methods to study the controls on elemental abundances in spores, characterize the elemental distribution of in spores, and to study elemental uptake by spores. Our work under this LDRD project attracted FBI and DHS funding for applied purposes.
Date: February 26, 2007
Creator: Weber, P K; Ghosal, S; Leighton, T J; Wheeler, K E & Hutcheon, I D
Partner: UNT Libraries Government Documents Department

Quantitative Analysis of Supported Membrane Composition using the NanoSIMS

Description: We have improved methods reported earlier [1] for sample preparation, imaging and quantifying components in supported lipid bilayers using high-resolution secondary ion mass spectrometry performed with the NanoSIMS 50. By selectively incorporating a unique stable isotope into each component of interest, a component-specific image is generated from the location and intensity of the unique secondary ion signals exclusively produced by each molecule. Homogeneous supported lipid bilayers that systematically varied in their isotopic enrichment levels were freeze-dried and analyzed with the NanoSIMS 50. The molecule-specific secondary ion signal intensities had an excellent linear correlation to the isotopically labeled lipid content. Statistically indistinguishable calibration curves were obtained using different sample sets analyzed months apart. Fluid bilayers can be patterned using lithographic methods and the composition of each corralled region varied systematically by simple microfluidic methods. The resulting composition variations can be imaged and quantified. This approach opens the possibility of imaging and quantifying the composition of microdomains within membranes, including protein components, without using bulky labels and with very high lateral resolution and sensitivity.
Date: August 28, 2005
Creator: Kraft, M; Foster, S; Marxer, C G; Weber, P; Hutcheon, I & Boxer, S
Partner: UNT Libraries Government Documents Department

Experimental study of radium partitioning between anorthite and melt at 1 atm

Description: We present the first experimental radium mineral/melt partitioning data, specifically between anorthite and a CMAS melt at atmospheric pressure. Ion microprobe measurement of coexisting anorthite and glass phases produces a molar D{sub Ra} = 0.040 {+-} 0.006 and D{sub Ra}/D{sub Ba} = 0.23 {+-} 0.05 at 1400 C. Our results indicate that lattice strain partitioning models fit the divalent (Ca, Sr, Ba, Ra) partition coefficient data of this study well, supporting previous work on crustal melting and magma chamber dynamics that has relied on such models to approximate radium partitioning behavior in the absence of experimentally determined values.
Date: March 8, 2007
Creator: Miller, S; Burnett, D; Asimow, P; Phinney, D & Hutcheon, I
Partner: UNT Libraries Government Documents Department

Towards consistent chronology in the early Solar System: high resolution 53Mn-53Cr chronometry for chondrules.

Description: New high-precision {sup 53}Mn-{sup 53}Cr data obtained for chondrules extracted from a primitive ordinary chondrite, Chainpur (LL3.4), define an initial {sup 53}Mn/{sup 55}Mn ratio of (5.1 {+-} 1.6) x 10{sup -6}. As a result of this downward revision from an earlier higher value of (9.4 {+-} 1.7) x 10{sup -6} for the same meteorite (Nyquist et al. 2001), together with an assessment of recent literature, we show that a consistent chronology with other chronometers such as the {sup 26}Al-{sup 26}Mg and {sup 207}Pb-{sup 206}Pb systems emerges in the early Solar System.
Date: May 2, 2007
Creator: Yin, Q; Jacobsen, B; Moynier, F & Hutcheon, I D
Partner: UNT Libraries Government Documents Department

Analysis of Savannah Survey Sediment Collections of 30 Sep 04

Description: This report summarizes laboratory radiochemical analyses of sediment samples collected by the Defense Threat Reduction Agency during the DoD Savannah Survey operations of Sep 04. The analytic goal was to determine if Wassaw Sound sediment collections of 30 Sep 04 display evidence for local anthropogenic uranium, as distinct from the recognized regional background stemming from the Savannah River Site (SRS). Radiochemical methods were selected to maximize detection sensitivity for such anthropogenic uranium. Within the suite of twelve collections, there would be evidence for a localized source if individual collections were to differ from the population as a whole. If in fact non-natural uranium were observed, definitive determination of whether the source was SRS effluent or a localized release would likely involve additional field sampling. These collections were logged by the LLNL Forensics Science Center, photographed, and laboratory chain-of-custody was begun. The inventory received at LLNL is reported in Table 1. The separate collections were not assigned any relative priority among them. LLNL has separately reviewed detailed records of the item in question, and determined what materials are involved and what radiochemical assays are of value. Attempting quantitative estimates of source-item material release, transport, and collection levels would be quite uncertain. Rather, present assays examine for departure from natural background isotopic compositions. To summarize the findings, analyses for all collections displayed natural uranium isotopic composition--considering the {sup 238}U/{sup 235}U and {sup 236}U/{sup 235}U ratios--within measurement uncertainties, which were quite low. No one collection or set of collections stood apart from the others in its uranium isotopes. These {sup 238}U/{sup 235}U data uncertainty levels also determined with 99.5% confidence (a three-standard-deviation determination) that no more than 0.46% of the total uranium present in the Savannah Survey collections could be depleted uranium. Based on gamma spectroscopy assays of {sup 137}Cs specific activity (Becquerels ...
Date: December 3, 2004
Creator: Wimer, N; Hutcheon, I; Esser, B & Ramon, E
Partner: UNT Libraries Government Documents Department

Impurity and laser-induced damage in the growth sectors of rapidly grown DKP crystals

Description: We report the experimental results of impurity contamination and laser-induced damage investigations on rapidly grown potassium dihydrogen phosphate (KDP) crystals. Using absorption spectroscopy and chemical analysis, we determined the impurity distribution in the different growing sectors of KDP single crystals. The level of impurity was dependent on starting materials and growth rate. We also studied influence of impurities on laser-induced damage in fast grown KDP. The laser damage threshold (LDT) in the impurity-rich prismatic sector is same as in the high purity pyramidal sector within experimental error. Meanwhile, the LDT at the boundary of the prismatic and pyramidal sectors is less than half of that in the bulk. Furthermore, we found that the thermal annealing of the crystal eliminated the weakness of this sector boundary and increased its LDT to the same level as in the bulk of the crystal. Result suggests that the laser damage occurred in the vicinity of a high; localized strain field.
Date: February 13, 1997
Creator: Yan, M.; Torres, R.; Runkel, M.; Woods, B.; Hutcheon, I.; Zaitseva, N. et al.
Partner: UNT Libraries Government Documents Department

Depth profiling of polishing-induced contamination on fused silica surfaces

Description: Laser-induced damage on optical surfaces is often associated with absorbing contaminants introduced by the polishing process. This is particularly the case for UV optics. Here secondary ion mass spectroscopy (SIMS) was used to measure depth profiles of finished process contamination on fused silica surfaces. Contaminants detected include the major polishing compound components (Ce or Zr from CeO2 or ZrO2), Al presently largely because of the use of Al2O3 in the final cleaning process (Fe, Cu,Cr) incorporated during the polishing step or earlier grinding steps. Depth profile data typically showed an exponential decay of contaminant concentration to a depth of 100-200 nm. This depth is consistent with a polishing redeposition layers formed during the chemo-mechanical polishing of fused silica. Peak contaminant levels are typically in the 10-100 ppm range, except for Al with exceeds 1000 ppm. A strong correlation has been shown between the presence of a gray haze damage morphology and the use of CeO2 polishing compound. No strong correlation was found however between high levels of Ce, or any other contaminant and the low damage threshold was observed. In fact one of the strongest indications of a correlation is between increased damage thresholds and increased Zr contamination. This suggests that the correlation between redeposition layer and laser damage threshold is not simple an absorbing contaminant issue.
Date: December 20, 1997
Creator: Kozlowski, M.R.; Carr, J.; Hutcheon, I,; Torres, R.; Sheehan, L. Camp, D. & Yan, M.
Partner: UNT Libraries Government Documents Department