DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers

Abstract

The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227Ac: grand-daughter nuclides in the 238U and 235U decay chains respectively. The 230Th-234U, 226Ra-238U, 231Pa-235U, and 227Ac-235U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226Ra-238U and 227Ac-235U chronometers and provide information about nuclide migration during uranium processing.

Authors:
 [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1241985
Report Number(s):
LLNL-JRNL-669502
Journal ID: ISSN 0236-5731; TRN: US1600477
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Radioanalytical and Nuclear Chemistry
Additional Journal Information:
Journal Volume: 307; Journal Issue: 3; Journal ID: ISSN 0236-5731
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND RUEL MATERIALS; 07 ISOTOPES AND RADIATION SOURCES; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; radiochemistry; age-dating; radium, actinium; uranium; nuclear forensics

Citation Formats

Kayzar, Theresa M., and Williams, Ross W.. Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers. United States: N. p., 2015. Web. doi:10.1007/s10967-015-4435-4.
Kayzar, Theresa M., & Williams, Ross W.. Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers. United States. https://doi.org/10.1007/s10967-015-4435-4
Kayzar, Theresa M., and Williams, Ross W.. Sat . "Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers". United States. https://doi.org/10.1007/s10967-015-4435-4. https://www.osti.gov/servlets/purl/1241985.
@article{osti_1241985,
title = {Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers},
author = {Kayzar, Theresa M. and Williams, Ross W.},
abstractNote = {The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227Ac: grand-daughter nuclides in the 238U and 235U decay chains respectively. The 230Th-234U, 226Ra-238U, 231Pa-235U, and 227Ac-235U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226Ra-238U and 227Ac-235U chronometers and provide information about nuclide migration during uranium processing.},
doi = {10.1007/s10967-015-4435-4},
journal = {Journal of Radioanalytical and Nuclear Chemistry},
number = 3,
volume = 307,
place = {United States},
year = {Sat Sep 26 00:00:00 EDT 2015},
month = {Sat Sep 26 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Production date determination of uranium-oxide materials by inductively coupled plasma mass spectrometry
journal, September 2007


235U–231Pa age dating of uranium materials for nuclear forensic investigations
journal, January 2013

  • Eppich, Gary R.; Williams, Ross W.; Gaffney, Amy M.
  • Journal of Analytical Atomic Spectrometry, Vol. 28, Issue 5
  • DOI: 10.1039/c3ja50041a

A new RaBa chromatographic separation and its application to Ra mass-spectrometric measurement in volcanic rocks
journal, June 1994


Age determination of uranium samples by inductively coupled plasma mass spectrometry using direct measurement and spectral deconvolution
journal, January 2010

  • Varga, Zsolt; Wallenius, Maria; Mayer, Klaus
  • Journal of Analytical Atomic Spectrometry, Vol. 25, Issue 12
  • DOI: 10.1039/c0ja00048e

Measurement of Femtogram Quantities of Protactinium in Silicate Rock Samples by Multicollector Inductively Coupled Plasma Mass Spectrometry
journal, July 2004

  • Regelous, Marcel; Turner, Simon P.; Elliott, Tim R.
  • Analytical Chemistry, Vol. 76, Issue 13
  • DOI: 10.1021/ac030374l

Nuclear Forensic Science: Correlating Measurable Material Parameters to the History of Nuclear Material
journal, October 2012

  • Mayer, Klaus; Wallenius, Maria; Varga, Zsolt
  • Chemical Reviews, Vol. 113, Issue 2
  • DOI: 10.1021/cr300273f

Evaluation of chronometers in plutonium age determination for nuclear forensics: What if the ‘Pu/U clocks’ do not match?
journal, July 2014

  • Sturm, M.; Richter, S.; Aregbe, Y.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 302, Issue 1
  • DOI: 10.1007/s10967-014-3294-8

Determination of radium isotope ratios and abundances in geological samples by thermal ionization mass spectrometry
journal, May 1991

  • Volpe, Alan M.; Olivares, Jose A.; Murrell, Michael T.
  • Analytical Chemistry, Vol. 63, Issue 9
  • DOI: 10.1021/ac00009a015

High Th/U ratios in subcontinental lithospheric mantle: mass spectrometric measurement of Th isotopes in Gaussberg lamproites
journal, July 1992


Development and validation of a methodology for uranium radiochronometry reference material preparation
journal, March 2012


An Inter-Laboratory Assessment of the Thorium Isotopic Composition of Synthetic and Rock Reference Materials
journal, March 2008


Improved techniques for high accuracy isotope ratio measurements of nuclear materials using thermal ionization mass spectrometry
journal, October 2003


Measurement of Femtogram Quantities of Protactinium in Silicate Rock Samples by Multicollector Inductively Coupled Plasma Mass Spectrometry
journal, December 2007

  • Regelous, Marcel; Turner, Simon; Elliott, Tim
  • Analytical Chemistry, Vol. 80, Issue 1
  • DOI: 10.1021/ac702316r

Works referencing / citing this record:

The application of radiochronometry during the 4th collaborative materials exercise of the nuclear forensics international technical working group (ITWG)
journal, February 2018

  • Kristo, Michael J.; Williams, Ross; Gaffney, Amy M.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 315, Issue 2
  • DOI: 10.1007/s10967-017-5680-5

Application of the 226Ra–230Th–234U and 227Ac–231Pa–235U radiochronometers to UF6 cylinders
journal, June 2018

  • Rolison, John M.; Williams, Ross W.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 317, Issue 2
  • DOI: 10.1007/s10967-018-5955-5

Improved protactinium spike calibration method applied to 231Pa–235U age-dating of certified reference materials for nuclear forensics
journal, August 2018

  • Treinen, Kerri C.; Gaffney, Amy M.; Rolison, John M.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 318, Issue 1
  • DOI: 10.1007/s10967-018-6149-x

An interlaboratory collaboration to determine consensus 231Pa/235U model ages of a uranium certified reference material for nuclear forensics
journal, February 2020

  • Kayzar-Boggs, Theresa M.; Treinen, Kerri C.; Okubo, Ayako
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 323, Issue 3
  • DOI: 10.1007/s10967-020-07030-x

A case study in plutonium radiochronometry using multiple isotope systems
journal, August 2018

  • Gaffney, Amy M.; Wimpenny, Josh B. N.; Parsons-Davis, Tashi
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 318, Issue 1
  • DOI: 10.1007/s10967-018-6131-7

Application of the 226Ra–230Th–234U and 227Ac–231Pa–235U radiochronometers to uranium certified reference materials
journal, November 2017

  • Rolison, John M.; Treinen, Kerri C.; McHugh, Kelly C.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 314, Issue 3
  • DOI: 10.1007/s10967-017-5619-x

Atomic spectrometry update: review of advances in the analysis of metals, chemicals and materials
journal, January 2017

  • Carter, Simon; Fisher, Andy; Gibson, Bridget
  • Journal of Analytical Atomic Spectrometry, Vol. 32, Issue 11
  • DOI: 10.1039/c7ja90046e

Evaluating uranium radiochronometry by single-collector mass spectrometry for nuclear forensics: a multi-instrument investigation
journal, October 2019

  • Treinen, Kerri C.; Samperton, Kyle M.; Lindvall, Rachel E.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 322, Issue 3
  • DOI: 10.1007/s10967-019-06832-y

Atomic spectrometry update: review of advances in the analysis of metals, chemicals and materials
journal, January 2018

  • Carter, Simon; Clough, Robert; Fisher, Andy
  • Journal of Analytical Atomic Spectrometry, Vol. 33, Issue 11
  • DOI: 10.1039/c8ja90039f

Atomic spectrometry update: review of advances in the analysis of metals, chemicals and materials
journal, January 2020

  • Carter, Simon; Clough, Robert; Fisher, Andy
  • Journal of Analytical Atomic Spectrometry, Vol. 35, Issue 11
  • DOI: 10.1039/d0ja90067b

Atomic spectrometry update. Review of advances in the analysis of metals, chemicals and materials
journal, January 2013

  • Carter, Simon; Fisher, Andy S.; Hinds, Michael W.
  • Journal of Analytical Atomic Spectrometry, Vol. 28, Issue 12
  • DOI: 10.1039/c3ja90051g