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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

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

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

Constraints on the Origin of Chondrules and CAIs from Short-Lived and Long-Lived Radionuclides

Description: The high time resolution Pb-Pb ages and short-lived nuclide based relative ages for CAIs and chondrules are reviewed. The solar system started at 4567.2 {+-} 0.6Ma inferred from the high precision Pb-Pb ages of CAIs. Time scales of CAIs ({le}0.1Myr), chondrules (1-3Myr), and early asteroidal differentiation ({ge}3Myr) inferred from {sup 26}Al relative ages are comparable to the time scale estimated from astronomical observations of young star; proto star, classical T Tauri star and week-lined T Tauri star, respectively. Pb-Pb ages of chondrules also indicate chondrule formation occur within 1-3 Myr after CAIs. Mn-Cr isochron ages of chondrules are similar to or within 2 Myr after CAI formation. Chondrules from different classes of chondrites show the same range of {sup 26}Al ages in spite of their different oxygen isotopes, indicating that chondrule formed in the localized environment. The {sup 26}Al ages of chondrules in each chondrite class show a hint of correlation with their chemical compositions, which implies the process of elemental fractionation during chondrule formation events.
Date: October 24, 2005
Creator: Kita, N. T.; Huss, G. R.; Tachibana, S.; Amelin, Y.; Nyquist, L. E. & Hutcheon, I. D.
Partner: UNT Libraries Government Documents Department

High resolution trace element and isotopic imaging of microbial systems by NanoSIMS

Description: The NanoSIMS 50 is the state of the art in high spatial resolution secondary ion mass spectrometry (SIMS), combining unprecedented spatial resolution (as good as 50 nm) with ultra-high sensitivity (minimum detection limit of {approx}200 atoms). The NanoSIMS has 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 provides a novel new approach to the study of microbial systems. We have applied our NanoSIMS to various microbial systems. We have analyzed sub-regions of bacterial cells, biofilms, and other associated materials to map trace element and isotopic ratios on a submicron scale. Growth and metabolism have been tracked using stable isotope labels. High resolution SIMS is particularly powerful when used in combination with other high resolution techniques, such as FIB and TEM. Examples will be presented to demonstrate the range of capabilities of this technique for microbial systems.
Date: September 8, 2005
Creator: Weber, P K; Fallon, S J; Pett-Ridge, J; Ghosal, S; Ramon, C E & Hutcheon, I D
Partner: UNT Libraries Government Documents Department

Membrane composition analysis by imaging mass spectrometry

Description: Membranes on solid supports offer an ideal format for imaging. Secondary ion mass spectrometry (SIMS) can be used to obtain composition information on membrane-associated components. Using the NanoSIMS50, images of composition variations in membrane domains can be obtained with a lateral resolution better than 100 nm. By suitable calibration, these variations in composition can be translated into a quantitative analysis of the membrane composition. Progress towards imaging small phase-separated lipid domains, membrane-associated proteins and natural biological membranes will be described.
Date: March 29, 2006
Creator: Boxer, S G; Kraft, M L; Longo, M; Hutcheon, I D & Weber, P K
Partner: UNT Libraries Government Documents Department

Renewed Search for FUN (Fractionated and Unidentified Nuclear Effects) in Primitive Chondrites

Description: Ca-Al-rich inclusions (CAIs) found in primitive chondrites record processes and conditions of the earliest solar system as they are the oldest known solid objects formed in the solar system [1,2]. CAIs with fractionation and unidentified nuclear anomalies (FUN CAIs; [3]) are very rare and thusfar found exclusively in CV carbonaceous chondrites (e.g., Allende and Vigarano)[4]. FUN CAIs are characterized by large nucleosynthetic anomalies in several elements (Ca, Ti, Si, Sr, Ba, Nd, and Sm), large mass-dependant isotope fractionation (Mg, Si, and O), and very little initial {sup 26}Al [4,5 and reference therein]. Formation of FUN CAIs by thermal processing of presolar dust aggregates prior to the injection of {sup 26}Al into the protoplanetary disk has been proposed. More recently [5] proposed that FUN CAIs formed from a protosolar molecular cloud after injection of {sup 26}Al but before {sup 26}Al and {sup 27}Al were completely homogenized. Therefore discovering more FUN CAIs to perform U-Pb and other short-lived chronometric dating will provide key constraints on the age of the solar system, the isotopic composition of the protosolar molecular cloud, the earliest stages of the thermal processing in the solar system and the timing of {sup 26}Al and other short-lived radionuclide injection into the nascent solar system. Most known FUN CAIs were discovered and studied > 30 yr ago, and their isotope ratios determined using thermal ionization mass spectrometry (TIMS). Most of these FUN CAIs were almost or entirely consumed during their respective analyses. [5] recently identified a new FUN CAI (NWA 779 KS-1) based on O and Mg isotope ratios determined by SIMS and MCICPMS, respectively. We have initiated a systematic search for FUN CAIs in primitive chondrites, taking advantage of the large mass-dependant Mg isotope effects known for FUN inclusions with little or no inferred {sup 26}Al. Our strategy is to ...
Date: April 7, 2011
Creator: Tollstrup, D L; Wimpenny, J B; Yin, Q -; Ebel, D S; Jacobsen, B & Hutcheon, I D
Partner: UNT Libraries Government Documents Department