Raman spectroscopy was used on 95 samples comprising mainly of uranium ore concentrates as well as some UF4 and UO2 samples, in order to classify uranium compounds for nuclear forensic purposes, for the first time. This technique was selected as it is non-destructive and rapid. The spectra obtained from 9 different classes of chemical compounds were subjected to multivariate data analysis such as principal component analysis (PCA), partial least square-discriminant analysis (PLS-DA) and Fisher Discriminant Analysis (FDA). These classes were ammonium diuranate (ADU), sodium diuranate (SDU), ammonium uranyl carbonate (AUC), uranyl hydroxide (UH), UO2, UO3, UO4, U3O8 and UF4. Unsupervised PCA of full spectra shows fairly good distinction among the classes with some overlaps observed with ADU and UH. These overlaps are also reflected in the poorer specificities determined by PLS-DA. Higher values of sensitivities and specificities of remaining compounds were obtained. Supervised FDA based on reduced dataset of only 40 variables shows similar results to that of PCA but with closer clustering of ADU, UH, SDU, AUC. As a rapid and non-destructive technique, Raman spectroscopy is useful and complements existing techniques in multi-faceted nuclear forensics.

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The identification of interdicted nuclear or radioactive materials requires the application of dedicated techniques. In this work, a new approach for characterizing powder of uranium ore concentrates (UOCs) is presented. It is based on image texture analysis and multivariate data modelling. 26 different UOCs samples were evaluated applying the Angle Measure Technique (AMT) algorithm to extract textural features on samples images acquired at 250× and 1000× magnification by Scanning Electron Microscope (SEM). At both magnifications, this method proved effective to classify the different types of UOC powder based on the surface characteristics that depend on particle size, homogeneity, and graininess and are related to the composition and processes used in the production facilities. Using the outcome data from the application of the AMT algorithm, the total explained variance was higher than 90% with Principal Component Analysis (PCA), while partial least square discriminant analysis (PLS-DA) applied only on the 14 black colour UOCs powder samples, allowed their classification only on the basis of their surface texture features (sensitivity>0.6; specificity>0.6). This preliminary study shows that this method was able to distinguish samples with similar composition, but obtained from different facilities. The mean angle spectral data obtained by the image texture analysis using the AMT algorithm can be considered as a specific fingerprint or signature of UOCs and could be used for nuclear forensic investigation.