• Mass Spectrometry Letters
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• v.7 no.4
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• pp.102-105
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• 2016

This study explored the feasibility of using a carburization technique to enhance the ion intensity of isotopic analysis of ultra-trace levels of uranium using thermal ionization mass spectrometry (TIMS). Prior to fixing uranium samples on TIMS filaments, graphite powder suspended in nitric acid was deposited on rhenium filaments. We observed an enhancement of $^{238}U^+$ intensity by a factor of two when carburization was used, and were able to roughly optimize the amount of graphite powder necessary for carburization. The positive shift in heating current when evaporating filaments upon carburization implies that uranium was chemically altered by carburization, when compared to normal fixation processes. The good agreement between our method and known standards down to an ultra-trace level shows that the proposed technique can be applied to isotopic uranium analysis down to abundances of ~10 pg.

• Mass Spectrometry Letters
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• v.7 no.3
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• pp.64-68
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• 2016

Scanning electron microscopy combined with thermal ionization mass spectrometry (SEM-TIMS) was used to determine the precise isotope ratios of ultra-trace levels of uranium contained in individual microparticles. An advanced multiple ion counter system consisting of three secondary ion multipliers and two compact discrete dynodes was used for complete simultaneous ion detection. For verification purposes, using TIMS with complete simultaneous measurement, isotopes were analyzed in 5 pg of uranium of a certified reference material. A microprobe in the SEM was used to transfer individual particles from a NUSIMEP-7 sample to TIMS filaments, which were then subjected to SEM-TIMS and complete simultaneous measurement. The excellent agreement in the resulting uranium isotope ratios with the certified NUSIMEP-7 values shows the validity of SEM-TIMS with complete simultaneous measurement for the analysis of uranium isotopes in individual particles. Further experimental study required for investigation of simultaneous measurement using the advanced multiple ion counter system is presented.

• Mass Spectrometry Letters
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• v.5 no.1
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• pp.12-15
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• 2014

Thermal ionization mass spectrometry (TIMS) was used to determine the concentration and isotope ratio of uranium contained in samples of soil and groundwater collected from Korea. Quantification of uranium in ground water samples was performed by isotope dilution mass spectrometry. A series of chemical treatment processes, including chemical separation using extraction chromatography, was applied to the soil samples to extract the uranium. No treatments other than filtration were applied to the groundwater samples. Isotopic analyses by TIMS showed that the isotope ratios of uranium in both the soil and water samples were indistinguishable from those of naturally abundant uranium. The concentration of uranium in the groundwater samples was within the U.S. acceptable standards for drinking water. These results demonstrate the utility of TIMS for monitoring uranium in environmental samples with high analytical reliability.

• Mass Spectrometry Letters
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• v.4 no.3
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• pp.51-54
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• 2013

Isotopic analysis using thermal ionization mass spectrometry coupled with scanning electron microscopy (SEM-TIMS) was performed to determine the isotopic ratios of uranium contained in micro-particles in the 6th Nuclear Signatures Interlaboratory Measurement Evaluation Programme (NUSIMEP-6) sample. Elemental analysis by energy dispersive X-ray spectroscopy (EDS) was conducted on uranium-bearing mirco-particles, which were transferred to rhenium filaments for TIMS loading using a micromanipulation system in a SEM. A multi-ion-counter system was utilized to detect the ion signals of the four isotopes of uranium simultaneously. The isotope ratios of uranium corrected by bracketing using a reference material showed excellent agreement with the certified values. The measurement accuracy for $n(^{234}U)/n(^{238}U)$ and (b) $n(^{235}U)/n(^{238}U)$ was 10% and 1%, respectively, which met the requirements for qalification for the NetWork of Analytical Laboratories (NWAL).

• Nuclear Engineering and Technology
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• v.52 no.7
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• pp.1532-1536
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• 2020

For ensuring nuclear safeguards, we report the analytical signal-detection performance of thermal ionization mass spectrometry (TIMS) with continuous heating for the measurement of isotopic ratios in samples containing ultra-trace amounts of uranium. As methods for detecting uranium signals, peak-jumping mode using a single detector and static mode using multiple detectors were examined with U100 (10% ²³⁵U-enriched) uranium standard samples in the femtogram-to-picogram range. Uranium isotope ratios, n(²³⁵U)/n(²³⁸U), were measured down to levels of 1 fg and 3 fg in static and peak-jumping modes, respectively, while n(²³⁴U)/n(²³⁸U) and n(²³⁶U)/n(²³⁸U) values were measured down to levels of 100 fg in both modes. In addition, the dependency of the ²³⁸U signal intensity on sample quantity exhibited similar tendencies in both modes. The precisions of the isotope ratios obtained in the static mode over all sample ranges used in this study were overall slightly higher than those obtained in peak-jumping mode. These results indicate that isotope ratio measurements by TIMS with continuous heating are almost independent of the detection method, i.e., peak-jumping mode or static mode, which is characteristic of isotope-ratio measurements using the TIMS method with continuous heating. TIMS with continuous heating is advantageous as it exhibits the properties of multiple detectors within a single detector, and is expected to be used in various fields in addition to ensuring nuclear safeguards.

• Mass Spectrometry Letters
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• v.1 no.1
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• pp.17-20
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• 2010

As background significantly affects measurement accuracy and a detection limit in determination of the trace amounts of uranium, it is necessary to minimize the impurities in the filaments used for thermal ionization mass spectrometry (TIMS). We have varied the degassing condition such as the heating currents and duration times to reduce the backgrounds from the filaments prepared with zone-refined rhenium tape. The most efficient degassing condition of the heating current and the duration time was determined as 3.5 A and 60 min, respectively. The TIMS measurement combined with the isotope dilution mass spectrometry (IDMS) technique showed that the uranium backgrounds were determined to be in a few fg level from blank rhenium filaments. The background minimized filaments were utilized to measure the uranium isotope ratios of a U030 (NIST) standard sample. The excellent agreement of the measurement with the certified isotope ratios showed that the degassing procedure optimized in this study efficiently reduced the impurity signals of uranium from blank rhenium filaments to a negligible level.

• Mass Spectrometry Letters
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• v.2 no.2
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• pp.57-60
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• 2011

As background significantly affects measurement accuracy and a detection limit in determination of the trace amounts of uranium, it is necessary to determine the impurities in the Lexan detector film for single particle measurements by thermal ionization mass spectrometry coupled with fission track technique (FT-TIMS). We have prepared various micro sizes of the blank Lexan detector film using a micromanipulation technique for uranium measurements by TIMS. Few tens of fg of uranium background with no remarkable dependency on the film sizes were observed in the blank Lexan films with the sizes from $50{\times}50\;{\mu}m^2$ to $300{\times}300\;{\mu}m^2$. Based on the determination of the uranium background in the Lexan film, any background correction is necessary in the isotopic analysis of a uranium single particle with micron sizes when the particle bearing Lexan film is dissected with less than $300{\times}300\;{\mu}m^2$ size. The isotopic analysis of a uranium particle in U030 standard material using TIMS was carried out to verify the applicability of the Lexan film to the single particle analysis with high accuracy and precision.

• Bulletin of the Korean Chemical Society
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• v.32 no.12
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• pp.4327-4331
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• 2011

A new method in thermal ionization mass spectrometry (TIMS) was developed to correct peak tailing backgrounds in the isotope ratio measurements of uranium in ultra trace levels for higher accuracy. Two different uranium standard reference materials (U005 and U030) were used to construct databases of signal intensities at mass 234 u and mass 236 u, which correspond to the two uranium minor isotopes, and signal intensity of $^{238}U$. Correlations between peak tailing backgrounds and $^{238}U$ were obtained by least-squares regression on calculated backgrounds at mass 234 u and mass 236 u with respect to the signal intensity of $^{238}U$ followed by separation of the peak tails of the two major isotopes of uranium ($^{235}U$ and $^{238}U$), which enables us to obtain a master equation for peak tailing background correction on all kinds of samples. Verification of the correction method was carried out using U010 and IRMM-040a.

• Journal of Radiation Protection and Research
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• v.43 no.3
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• pp.120-123
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• 2018

Background: Analysis of enrichment of $UO_2$ is important to verify the information declared by the license-holders. The redundancy methods are required to guarantee the analysis result. Korea Institute of Nuclear Nonproliferation and Control (KINAC) used to analyze it with alpha spectrometry and consign to Korea Basic Science Institute (KBSI) Thermal Ionization Mass Spectrometry (TIMS). This article evaluated the similarity of the results with two methods and derive correlation equation. It could be compared to the results measured by TIMS running by KBSI. Materials and Methods: There are not many certified materials for the uranium enrichment value. Therefore, 34 uranium pellets, which have the wide range of uranium enrichment from 0.21 to 4.69 wt%, were used for the experiments by the alpha spectrometry and the TIMS. Results and Discussion: The study shows there are the tendency of analyzed enrichment by each equipment. It shows uranium enrichment with alpha spectrometry evaluated 17% higher than that with TIMS on average. The regression equations were also derived in case the similarity between the two results with two methods is lower than predicted. Two experiments were designed to compare the effect of number of samples. The $R^2$ was 0.9977 with 34 pellets. It shows the equation is appropriate to predict the enrichment values by TIMS with that of alpha spectrometry. The $R^2$ was 0.9858 with four pellets for ten times. The $R^2$ decreased while the number of samples increased. The discrepancy between the lowest and highest enrichment seems to be one of the reason for it. Conclusion: KINAC expects the first equation with 34 samples is useful to predict the result with TIMS, the redundancy method, based on the alpha spectrometry. The extra samples are necessary to collect if the enrichment value analyzed by TIMS is lower than the value predicted with the equation. Further study would be followed related to the impact of the peak counts for each uranium isotopes, sample amount and number of experiments when TIMS established in KINAC by the end of 2018.

• Nuclear Engineering and Technology
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• v.50 no.1
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• pp.140-144
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• 2018

Isotopic analyses of plutonium and low-enriched uranium mixtures with particle sizes of $0.6-3.3{\mu}m$ were performed using thermal ionization mass spectrometry with a continuous heating method to verify its effectiveness for the accurate analysis of minor isotopes without sample pretreatment. The mixed particles used in this study were prepared from a mixed solution of plutonium (SRM 947) and uranium (U010, $^{235}U$ 1% enriched) reference materials. The isotope ratios for plutonium in the individual mixed particles, including $^{238}Pu/^{239}Pu$, $^{241}Pu/^{239}Pu$ as well as $^{240}Pu/^{239}Pu$, and $^{242}Pu/^{239}Pu$, were in good agreement with the certified values despite the isobaric interference of $^{238}U$ and $^{241}Am$. The isotope ratios for uranium in the mixed particles also agreed well with the certified values within the range of error. However, the isotope ratios for minor isotopes, such as $^{234}U$ and $^{236}U$, in the particles with diameters of less than approximately $1.8{\mu}m$ could not be measured because numbers of $^{234}U$ and $^{236}U$ atoms in analyzed particles are too low. These results indicate that thermal ionization mass spectrometry with a continuous heating method is applicable for the analysis of trace amounts of plutonium isotopes, including $^{238}Pu$ and $^{241}Pu$, despite the presence of the respective isobars $^{238}U$ and $^{241}Am$ in the microsamples.