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

Title: Analytical comparisons of handheld LIBS and XRF devices for rapid quantification of gallium in a plutonium surrogate matrix

Journal Article · · Journal of Analytical Atomic Spectrometry
DOI:https://doi.org/10.1039/d1ja00404b· OSTI ID:2202628

This work compares a portable laser-induced breakdown spectroscopy (LIBS) analyzer to a portable X-ray fluorescence (XRF) device for quantification of gallium (Ga) in a plutonium surrogate matrix of cerium (Ce) for the first time. Calibration methods are developed with spectra of Ce–Ga samples from both devices. Here, metrics such as limit of detection (LoD) and mean average percent error (MAPE) are examined to evaluate calibration performance. While the portable LIBS device can yield a nearly instantaneous analytical measurement, its accuracy is hampered by self-absorption. By employing a self-absorption correction and increasing gating delay, LIBS calibrations with errors in the low single percents and LoDs of 0.1% Ga were constructed. The XRF device produces calibrations with superlative sensitivity, yielding LoDs for gallium in the low tens of parts-per-million (ppm), two orders of magnitude lower than the corrected LIBS models. However, a clear trade-off of measurement fidelity is established between the instantaneous analysis of the LIBS device and the minutes-long XRF measurement yielding superior detection limits.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); Defense Threat Reduction Agency (DTRA)
Grant/Contract Number:
89233218CNA000001
OSTI ID:
2202628
Report Number(s):
LA-UR-21-29174
Journal Information:
Journal of Analytical Atomic Spectrometry, Vol. 37, Issue 5; ISSN 0267-9477
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Analysis of material collected on swipes using laser-induced breakdown spectroscopy journal January 2010
Portable XRF analysis of archaeological sediments and ceramics journal January 2015
Field portable XRF analysis of environmental samples journal May 2001
Lithium ion detection in liquid with low detection limit by laser-induced breakdown spectroscopy journal January 2019
Analysis of Rare Earth Elements in Uranium Using Handheld Laser-Induced Breakdown Spectroscopy (HH LIBS) journal May 2018
Measurement of electron density and temperature from laser-induced nitrogen plasma at elevated pressure (1–6 bar) journal January 2019
Comparison of machine learning techniques to optimize the analysis of plutonium surrogate material via a portable LIBS device journal January 2021
A novel approach to sensitivity evaluation of laser-induced breakdown spectroscopy for rare earth elements determination journal January 2016
Determination of uranium concentration in an ore sample using laser-induced breakdown spectroscopy journal August 2012
On the performance of laser-induced breakdown spectroscopy for quantitative analysis of minor and trace elements in glass journal January 2015
Elemental characterization of nuclear materials using total reflection X-ray fluorescence spectrometry journal July 2019
A portable XRF spectrometer for non-destructive analyses in archaeometry
  • Longoni, A.; Fiorini, C.; Leutenegger, P.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 409, Issue 1-3 https://doi.org/10.1016/S0168-9002(98)00113-2
journal May 1998
Laser-Induced Breakdown Spectroscopy (LIBS), Part II: Review of Instrumental and Methodological Approaches to Material Analysis and Applications to Different Fields journal April 2012
Multivariate approach to the chemical mapping of uranium in sandstone-hosted uranium ores analyzed using double pulse Laser-Induced Breakdown Spectroscopy journal September 2016
Characterization of Cast Metals with Probability Distribution Functions journal January 1998
Mechanisms and efficient elimination approaches of self-absorption in LIBS journal January 2019
Mapping of Uranium in Surrogate Nuclear Debris Using Laser-Induced Breakdown Spectroscopy (LIBS) journal March 2019
Multi-element analysis of soil and sediment by ICP-MS after a microwave assisted digestion method journal January 2000
Recent advances in inductively coupled plasma optical emission spectrometry journal January 2017
Investigation of the self-absorption effect using time-resolved laser-induced breakdown spectroscopy journal February 2019
Effect of self-absorption correction on LIBS measurements by calibration curve and artificial neural network journal July 2013
Laser-Induced Breakdown Spectroscopy (LIBS), Part I: Review of Basic Diagnostics and Plasma—Particle Interactions: Still-Challenging Issues within the Analytical Plasma Community journal December 2010
Towards the determination of the geographical origin of yellow cake samples by laser-induced breakdown spectroscopy and chemometrics journal January 2009
Detection of uranyl fluoride and sand surface contamination on metal substrates by hand-held laser-induced breakdown spectroscopy journal January 2017
A review of the current analytical approaches for evaluating, compensating and exploiting self-absorption in Laser Induced Breakdown Spectroscopy journal July 2020
Quantitative Analysis of Cerium-Gallium Alloys Using a Hand-Held Laser Induced Breakdown Spectroscopy Device journal August 2019
Identification of a physical metallurgy surrogate for the plutonium—1 wt. % gallium alloy conference January 2000
Analysis of plutonium oxide surrogate residue using laser-induced breakdown spectroscopy journal September 2008
Application of XRF and field portable XRF for environmental analysis journal January 2004
Phonon and magnetic structure in δ-plutonium from density-functional theory journal October 2015
Rapid quantitative analysis of trace elements in plutonium alloys using a handheld laser-induced breakdown spectroscopy (LIBS) device coupled with chemometrics and machine learning journal January 2021
Determination of thorium and uranium in solution by laser-induced breakdown spectrometry journal January 2008
Quantitative analysis of common elements in steel using a handheld μ-LIBS instrument journal January 2017
Simultaneous LIBS signal and plasma density measurement for quantitative insight into signal instability at elevated pressure journal January 2018
Multivariate Analysis of Laser-Induced Breakdown Spectroscopy Spectra of Soil Samples journal January 2010
Evaluation of self-absorption coefficients of aluminum emission lines in laser-induced breakdown spectroscopy measurements journal December 2005
Multivariate analysis of laser-induced breakdown spectroscopy chemical signatures for geomaterial classification journal October 2009
Improving precision of X-ray fluorescence analysis of lanthanide mixtures using partial least squares regression journal November 2015
Capabilities of high resolution ICP-OES for plutonium isotopic analysis journal March 2016