skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Development of small particle speciation for nuclear forensics by soft X-ray scanning transmission spectromicroscopy

Journal Article · · Analyst
DOI:https://doi.org/10.1039/c7an01838j· OSTI ID:1513794
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [3];  [1];  [5];  [1]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source

Synchrotron radiation spectromicroscopy provides a combination of submicron spatial resolution and chemical sensitivity that is well-suited to analysis of heterogeneous nuclear materials. The chemical and physical characteristics determined by scanning transmission X-ray microscopy (STXM) are complementary to information obtained from standard radiochemical analysis methods. In addition, microscopic quantities of radioactive material can be characterized rapidly by STXM with minimal sample handling and intrusion, especially in the case of particulate materials. The STXM can accommodate a diverse range of samples including wet materials, complex mixtures, and small quantities of material contained in a larger matrix. In these cases, the inventory of species present in a sample is likely to carry information on its process history; STXM has the demonstrated capability to identify contaminants and sample matrices. Operating in the soft X-ray regime provides particular sensitivity to the chemical state of specimens containing low-Z materials, via the K-edges of light elements. In this paper, recent developments in forensics-themed spectromicroscopy, sample preparation, and data acquisition methods at the Molecular Environmental Science Beamline 11.0.2 of the Advanced Light Source are described. Results from several initial studies are presented, demonstrating the capability to identify the distribution of the species present in heterogeneous uranium-bearing materials. Finally, future opportunities for STXM forensic studies and potential methodology development are discussed.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; AC52-07NA27344
OSTI ID:
1513794
Alternate ID(s):
OSTI ID: 1438649
Report Number(s):
LLNL-JRNL-704342; ANALAO; ark:/13030/qt2c86203k
Journal Information:
Analyst, Vol. 143, Issue 6; ISSN 0003-2654
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

References (54)

Electronic structure and O K-edge XAS spectroscopy of U3O8 journal June 2014
Trinitite-the atomic rock journal September 2010
Radionuclide Fractionation in Bomb Debris: The fractionation systematics for high-yield bursts at sea-water and coral surfaces are delineated journal June 1961
Trinitite redux: Mineralogy and petrology journal February 2015
Sourcing of Copper and Lead within Red Inclusions from Trinitite Postdetonation Material journal May 2015
Probing Surface Oxidation of Reduced Uranium Dioxide Thin Film Using Synchrotron Radiation journal June 2007
Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing journal May 2016
Identification of Uranyl Minerals Using Oxygen K-Edge X-Ray Absorption Spectroscopy journal March 2015
The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide: A high resolution XPS study journal February 2007
Nuclear forensic investigations: Two case studies journal January 2006
Nuclear forensic investigations with a focus on plutonium journal October 2007
Automated Analysis of SEM X-Ray Spectral Images: A Powerful New Microanalysis Tool journal January 2003
X-ray absorption fine structure of aged, Pu-doped glass and ceramic waste forms journal April 1998
Use of Secondary Ion Mass Spectrometry in Nuclear Forensic Analysis for the Characterization of Plutonium and Highly Enriched Uranium Particles journal July 1999
Cluster analysis of soft X-ray spectromicroscopy data journal July 2004
Microanalytical X-ray Imaging of Depleted Uranium Speciation in Environmentally Aged Munitions Residues journal January 2014
Uranium co-precipitation with iron oxide minerals journal October 2002
The state of nuclear forensics journal January 2013
Development of a SIMS Method for Isotopic Measurements in Nuclear Forensic Applications journal May 2002
Soft X-ray scanning transmission X-ray microscopy (STXM) of actinide particles journal July 2005
Compositional dependence of redox equilibria in sodium silicate glasses journal November 1994
When the dust settles: stable xenon isotope constraints on the formation of nuclear fallout journal November 2014
In-situ Scanning Transmission X-Ray Microscopy of Catalytic Solids and Related Nanomaterials journal March 2010
Evolution of the uranium local environment during alteration of SON68 glass journal March 2002
Analytical Atomic Spectrometry for Nuclear Forensics journal August 2005
Lead Isotopic Composition of Trinitite Melt Glass: Evidence for the Presence of Canadian Industrial Lead in the First Atomic Weapon Test journal July 2013
Near-edge x-ray-absorption fine structure in uranium compounds journal February 1987
Nuclear forensics in law enforcement applications journal September 1998
Quantification of the ferric/ferrous iron ratio in silicates by scanning transmission X-ray microscopy at the Fe L2,3 edges journal June 2013
Atomic radiative and radiationless yields for K and L shells journal April 1979
Surface reactions of uranium oxide powder, thin films and single crystals journal March 2010
Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia journal January 2015
Interferometer-controlled scanning transmission X-ray microscopes at the Advanced Light Source journal February 2003
Oxidation and Hydration of U 3 O 8 Materials Following Controlled Exposure to Temperature and Humidity journal April 2015
A detailed geochemical investigation of post-nuclear detonation trinitite glass at high spatial resolution: Delineating anthropogenic vs. natural components journal February 2014
Postdetonation nuclear debris for attribution journal November 2010
The Use of SIMS and SEM for the Characterization of Individual Particles with a Matrix Originating from a Nuclear Weapon journal May 2007
The chemistry of uranium in glass-forming aluminosilicate melts journal May 1983
Possible Bose-condensate behavior in a quantum phase originating in a collective excitation in the chemically and optically doped Mott-Hubbard system UO 2 + x journal September 2013
Nuclear forensics—a methodology providing clues on the origin of illicitly trafficked nuclear materials journal January 2005
Constraints on fallout melt glass formation from a near-surface nuclear test journal July 2014
Image Super-Resolution Using Deep Convolutional Networks journal February 2016
Advances in the Detection of As in Environmental Samples Using Low Energy X-ray Fluorescence in a Scanning Transmission X-ray Microscope: Arsenic Immobilization by an Fe(II)-Oxidizing Freshwater Bacteria journal February 2012
Focused Ion Beam Microscopy and Micromachining journal May 2007
Isotopic Fingerprinting of the World’s First Nuclear Device Using Post-Detonation Materials journal March 2013
SIMS Analysis of Uranium and Actinides in Microparticles of Different Origin journal April 2004
Nuclear forensic analysis of an unknown uranium ore concentrate sample seized in a criminal investigation in Australia journal July 2014
New evidence for 5f covalency in actinocenes determined from carbon K-edge XAS and electronic structure theory journal January 2014
Ligand K-edge X-ray absorption spectroscopy: covalency of ligand–metal bonds journal January 2005
Nuclear Forensic Science: Correlating Measurable Material Parameters to the History of Nuclear Material journal October 2012
Plutonium Transport in the Environment journal June 2012
Properties of redox ions in glasses: An interdisciplinary perspective journal October 1980
Near-edge x-ray-absorption fine structure in uranium compounds text January 1987
X-Ray Absorption Fine Structure of Aged, Pu-Doped Glass and Ceramic Waste Forms journal January 1997

Cited By (5)

Atomic spectrometry update: review of advances in elemental speciation journal January 2019
Atomic Spectrometry Update: review of advances in elemental speciation journal January 2018
Atomic Spectrometry Update: review of advances in elemental speciation journal January 2016
Atomic spectrometry update: review of advances in elemental speciation journal January 2017
Atomic spectrometry update: review of advances in elemental speciation journal January 2020

Figures / Tables (7)