A novel isotope analysis of oxygen in uranium oxides: comparison of secondary ion mass spectrometry, glow discharge mass spectrometry and thermal ionization mass spectrometry

The natural variation of the oxygen isotopic composition is used among geologists to determine paleotemperatures and the origin of minerals. In recent studies, oxygen isotopic composition has been recognized as a possible tool for identification of the origin of seized uranium oxides in nuclear forensic science. In the last 10 years, great effort has been made to develop new direct and accurate n(18O)/n(16O) measurements methods. Traditionally, n(18O)/n(16O) analyses are performed by gas mass spectrometry. In this work, a novel oxygen isotope analysis by thermal ionization mass spectrometry (TIMS), using metal oxide ion species (UO+), is compared to the direct methods: glow discharge mass spectrometry (GDMS) and secondary ion mass spectrometry (SIMS). Because of the possible application of the n(18O)/n(16O) ratio in nuclear forensics science, the samples were solid, pure UO2 or U3O8 particles. The precision achieved using TIMS analysis was 0.04%, which is similar or even better than the one obtained using the SIMS technique (0.05%), and clearly better if compared to that of GDMS (0.5%). The samples used by TIMS are micrograms in size. The suitability of TIMS as a n(18O)/n(16O) measurement method is verified by SIMS measurements. In addition, TIMS results have been confirmed by characterizing the n(18O)/n(16O) ratio of UO2 sample also by the traditional method of static vacuum mass spectrometry at the University of Chicago.