Determination of isotope ratios using Laser-Induced Breakdown Spectroscopy in ambient air at atmospheric pressure for nuclear forensics

Abstract

Laser-Induced Breakdown Spectroscopy (LIBS) is currently a subject of great interest in spectroscopy and is being considered for the design of a field portable unit for nuclear safeguard inspection, because it allows a high level of portability and versatility while identifying the elements and materials of interest. Field portable technologies and methods are sought to provide simple, inexpensive, and fast analysis of materials in the mining, construction, and other industries. However, the level of portability needed for this particular application imposes some restrictions on the choice of many of the core components used in a low cost LIBS handheld sensor. This means that relatively low-performance components, such as a low-energy laser source and a low cost, low resolution spectrometer, must be considered to fulfil these conditions. In addition, the market price of such a portable device should be as low as possible to increase the breadth of potential end users and allow the deployment of multiple units for security enhancement. The present paper describes the determination of isotope ratios using Laser-Induced Breakdown Spectroscopy in air at atmospheric pressure for partially resolved uranium-235/uranium-238 and hydrogen/deuterium isotope shift lines in such conditions. Using a Partial Least Square (PLS1) regression, it is possible to build a model that enables the accurate determination of the isotopic ratio under conditions where the application of traditional univariate approaches for hydrogen and uranium would not be achievable without the use of ultra high resolution spectrometer. In addition, the application of PLS1 regression to determine the uranium-235/uranium-238 and deuterium/hydrogen isotopic ratios between 0 and 1 mass fraction was also successfully demonstrated. The performance obtained with such a LIBS sensor configuration demonstrates the possibility of integrating all of the required components in a small portable handheld system.