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Title: A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS)

Abstract

We are developing highly sensitive, highly discriminating laser-based techniques for rapid determination of isotopic compositions. Rapid command of such information is critical to assessment of the origin and history of nuclear materials, particularly in post-detonation scenarios.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
957166
Report Number(s):
LLNL-TR-413804
TRN: US1000605
DOE Contract Number:
W-7405-ENG-48
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; 36 MATERIALS SCIENCE; 42 ENGINEERING; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; IONIZATION; MASS SPECTROSCOPY; RESONANCE; SAMPLE PREPARATION; URANIUM ISOTOPES

Citation Formats

Knight, K B, Hutcheon, I D, Isselhardt, B H, Savina, M R, and Prussin, S G. A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS). United States: N. p., 2009. Web. doi:10.2172/957166.
Knight, K B, Hutcheon, I D, Isselhardt, B H, Savina, M R, & Prussin, S G. A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS). United States. doi:10.2172/957166.
Knight, K B, Hutcheon, I D, Isselhardt, B H, Savina, M R, and Prussin, S G. Mon . "A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS)". United States. doi:10.2172/957166. https://www.osti.gov/servlets/purl/957166.
@article{osti_957166,
title = {A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS)},
author = {Knight, K B and Hutcheon, I D and Isselhardt, B H and Savina, M R and Prussin, S G},
abstractNote = {We are developing highly sensitive, highly discriminating laser-based techniques for rapid determination of isotopic compositions. Rapid command of such information is critical to assessment of the origin and history of nuclear materials, particularly in post-detonation scenarios.},
doi = {10.2172/957166},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Jun 08 00:00:00 EDT 2009},
month = {Mon Jun 08 00:00:00 EDT 2009}
}

Technical Report:

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  • With support provided by the LLNL Accelerator Mass Spectrometry Laboratory, the UCR Radiocarbon Laboratory continued its studies involving sample pretreatment and target preparation for both AMS radiocarbon ({sup 14}C) and radiocalcium ({sup 41}Ca) involving applications to archaeologically -- and paleoanthropologically- related samples. With regard to AMS {sup 14}C-related studies, we have extended the development of a series of procedures which have, as their initial goal, the capability to combust several hundred microgram amounts of a chemically-pretreated organic sample and convert the resultant CO{sub 2} to graphitic carbon which will consistently yield relatively high {sup 13}C{sup {minus}} ion currents and blanksmore » which will yield, on a consistent basis, {sup 14}C count rates at or below 0.20% modern, giving an 2 sigma age limit of >50,000 yr BP.« less
  • With support provided by the LLNL Accelerator Mass Spectrometry Laboratory, the UCR Radiocarbon Laboratory continued its studies involving sample pretreatment and target preparation for both AMS radiocarbon ({sup 14}C) and radiocalcium ({sup 41}Ca) involving applications to archaeologically -- and paleoanthropologically- related samples. With regard to AMS {sup 14}C-related studies, we have extended the development of a series of procedures which have, as their initial goal, the capability to combust several hundred microgram amounts of a chemically-pretreated organic sample and convert the resultant CO{sub 2} to graphitic carbon which will consistently yield relatively high {sup 13}C{sup {minus}} ion currents and blanksmore » which will yield, on a consistent basis, {sup 14}C count rates at or below 0.20% modern, giving an 2 sigma age limit of >50,000 yr BP.« less
  • The cw laser RIMS approach has been demonstrated to accurately measure large Lu isotope ratios and detect small levels of minor isotopes even in the presence of isobaric interferences. The same approach can also be used to obtain high resolution optical spectra of rare isotopes. For elements with higher ionization potentials (e.g., Tc), multicolor ionization schemes are necessary for cw RIMS measurements. Two-color RIMS spectra of Tc using pulsed lasers illustrate the feasibility of this approach. For any element, the sensitivity and selectivity of RIMS can be limited by the efficiency of ground state atom production in the sample volatilizationmore » step.« less
  • Progress on investigations to improve precision on mass spectrometric isotopic ratio measurements is reported. A detailed set of intructions as submitted to ASTM Committee C-26.05 on the rapid preparation and analysis of uranium and plutonium samples mass spectrometrically by the resin bead technique is also presented. This report contains information on two separate topics: one is a progress report on the International Safeguards Project Office A.82 in which we investigated various means of obtaining better precision on mass spectrometric isotopic ratio measurements. The idea investigated most thoroughly was the use of a two-filament source configuration on a pulse-counting mass spectrometer;more » our conclusion was that better results could be obtained with commercially available source systems. ORNL has purchased a turret source for evaluation on the two stage mass spectrometer. The second part of this report is a copy of the resin bead mass spectrometric procedure wd have submitted to ASTM for consideration for inclusion in their standard practice manual. This is a detailed, step-by-step description of uranium and plutonium sample preparation and analysis using the rapid bulk resin bead technique.« less
  • The precise and accurate determination of isotopic composition in nuclear forensic samples is vital for assessing origin, intended use and process history. Thermal ionization mass spectrometry (TIMS) is widely accepted as the gold standard for high performance isotopic measurements and has long served as the workhorse in the isotopic ratio determination of nuclear materials. Nuclear forensic and safeguard specialists have relied heavily on such methods for both routine and atypical e orts. Despite widespread use, TIMS methods for the assay of actinide systems continue to be hindered by poor ionization e ciency, often less than tenths of a percent; themore » majority of a sample is not measured. This represents a growing challenge in addressing nextgeneration nuclear detection needs by limiting the ability to analyze ultratrace quantities of high priority elements that could potentially provide critical nuclear forensic signatures. Porous ion emitter (PIE) thermal ion sources were developed in response to the growing need for new TIMS ion source strategies for improved ionization e ciency, PIEs have proven to be simple to implement, straightforward approach to boosting ion yield. This work serves to expand the use of PIE techniques for the analysis of trace quantities of plutonium and americium. PIEs exhibited superior plutonium and americium ion yields when compared to direct lament loading and the resin bead technique, one of the most e cient methods for actinide analysis, at similar mass loading levels. Initial attempts at altering PIE composition for the analysis of plutonium proved to enhance sample utilization even further. Preliminary investigations of the instrumental fractionation behavior of plutonium and uranium analyzed via PIE methods were conducted. Data collected during these initial trial indicate that PIEs fractionate in a consistent, reproducible manner; a necessity for high precision isotope ratio measurements. Ultimately, PIEs methods were applied for the age determination of various uranium isotopic standards. PIEs did not exhibit signi cant advantages for the determination of model ages when compared to traditional laments; however, this trial was able to provide valuable insight for guiding future investigations.« less