• Nuclear Engineering and Technology
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• v.51 no.2
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• pp.384-393
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• 2019

An experimental validation of a nuclear forensics methodology for the source reactor-type discrimination of separated weapons-useable plutonium is presented. The methodology uses measured values of intra-element isotope ratios of plutonium and fission product contaminants. MCNP radiation transport codes were used for various reactor core modeling and fuel burnup simulations. A reactor-dependent library of intra-element isotope ratio values as a function of burnup and time since irradiation was created from the simulation results. The experimental validation of the methodology was achieved by performing two low-burnup experimental irradiations, resulting in distinct fuel samples containing sub-milligram quantities of weapons-useable plutonium. The irradiated samples were subjected to gamma and mass spectrometry to measure several intra-element isotope ratios. For each reactor in the library, a maximum likelihood calculation was utilized to compare the measured and simulated intra-element isotope ratio values, producing a likelihood value which is proportional to the probability of observing the measured ratio values, given a particular reactor in the library. The measured intra-element isotope ratio values of both irradiated samples and its comparison with the simulation predictions using maximum likelihood analyses are presented. The analyses validate the nuclear forensics methodology developed.

• Mass Spectrometry Letters
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• v.7 no.2
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• pp.31-40
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• 2016

The analysis of nuclear materials and environmental samples is an important issue in nuclear safeguards and nuclear forensics. An analysis technique for safeguard samples has been developed for the detection of undeclared nuclear activities and verification of declared nuclear activities, while nuclear forensics has been developed to trace the origins and intended use of illicitly trafficked nuclear or radioactive materials. In these two analytical techniques, mass spectrometry has played an important role in determining the isotope ratio of various nuclides, contents of trace elements, and production dates. These two techniques typically use similar analytical instruments, but the analytical procedure and the interpretation of analytical results differ depending on the analytical purpose. The isotopic ratio of the samples is considered the most important result in an environmental sample analysis, while age dating and impurity analysis may also be important for nuclear forensics. In this review, important aspects of these techniques are compared and the role of mass spectrometry, along with recent progress in related technologies, are discussed.

• Nuclear Engineering and Technology
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• v.51 no.5
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• pp.1355-1364
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• 2019

A recently published nuclear forensics methodology for source discrimination of separated weapons-grade plutonium utilizes intra-element isotope ratios and a maximum likelihood formulation to identify the most likely source reactor-type, fuel burnup and time since irradiation of unknown material. Sensitivity studies performed here on the effects of random measurement error and the uncertainty in intra-element isotope ratio values show that different intra-element isotope ratios have disproportionate contributions to the determination of the reactor parameters. The methodology is robust to individual errors in measured intra-element isotope ratio values and even more so for uniform systematic errors due to competing effects on the predictions from the selected intra-element isotope ratios suite. For a unique sample-model pair, simulation uncertainties of up to 28% are acceptable without impeding successful source-reactor discrimination. However, for a generic sample with multiple plausible sources within the reactor library, uncertainties of 7% or less may be required. The results confirm the critical role of accurate reactor core physics, fuel burnup simulations and experimental measurements in the proposed methodology where increased simulation uncertainty is found to significantly affect the capability to discriminate between the reactors in the library.

• Nuclear Engineering and Technology
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• v.50 no.6
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• pp.820-828
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• 2018

The growing nuclear threat has amplified the need for developing diverse and accurate nuclear forensics analysis techniques to strengthen nuclear security measures. The work presented here is part of a research effort focused on developing a methodology for reactor-type discrimination of weapons-grade plutonium. To verify the developed methodology, natural $UO_2$ fuel samples were irradiated in a thermal neutron spectrum at the University of Missouri Research Reactor (MURR) and produced approximately $20{\mu}g$ of weapons-grade plutonium test material. Radiation transport simulations of common thermal reactor types that can produce weapons-grade plutonium were performed, and the results are presented here. These simulations were needed to verify whether the plutonium produced in the natural $UO_2$ fuel samples during the experimental irradiation at MURR was a suitable representative to plutonium produced in common thermal reactor types. Also presented are comparisons of fission product and plutonium concentrations obtained from computational simulations of the experimental irradiation at MURR to the nondestructive and destructive measurements of the irradiated natural $UO_2$ fuel samples. Gamma spectroscopy measurements of radioactive fission products were mostly within 10%, mass spectroscopy measurements of the total plutonium mass were within 4%, and mass spectroscopy measurements of stable fission products were mostly within 5%.

• Proceedings of the Korean Radioactive Waste Society Conference
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• 2018.11a
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• pp.55-56
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• 2018

• Journal of Radiation Industry
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• v.17 no.4
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• pp.345-357
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• 2023

Nuclear forensics has been understood as a mendatory component in the international society for nuclear material control and non-proliferation verification. Radiochronometry of nuclear activities for nuclear forensics are decay series characteristics of nuclear materials and the Bateman equation to estimate when nuclear materials were purified and produced. Radiochronometry values have uncertainty of measurement due to the uncertainty factors in the estimation process. These uncertainties should be calculated using appropriate evaluation methods that are representative of the accuracy and reliability. The IAEA, US, and EU have been researched on radiochronometry and uncertainty of measurement, although the uncertainty calculation method using the Bateman equation is limited by the underestimation of the decay constant and the impossibility of estimating the age of more than one generation, so it is necessary to conduct uncertainty calculation research using computer simulation such as Monte Carlo method. This highlights the need for research using computational simulations, such as the Monte Carlo method, to overcome these limitations. In this study, we have analyzed mathematical models and the LHS (Latin Hypercube Sampling) methods to enhance the reliability of radiochronometry which is to develop an uncertainty algorithm for nuclear material radiochronometry using Bateman Equation. We analyzed the LHS method, which can obtain effective statistical results with a small number of samples, and applied it to algorithms that are Monte Carlo methods for uncertainty calculation by computer simulation. This was implemented through the MATLAB computational software. The uncertainty calculation model using mathematical models demonstrated characteristics based on the relationship between sensitivity coefficients and radiative equilibrium. Computational simulation random sampling showed characteristics dependent on random sampling methods, sampling iteration counts, and the probability distribution of uncertainty factors. For validation, we compared models from various international organizations, mathematical models, and the Monte Carlo method. The developed algorithm was found to perform calculations at an equivalent level of accuracy compared to overseas institutions and mathematical model-based methods. To enhance usability, future research and comparisons·validations need to incorporate more complex decay chains and non-homogeneous conditions. The results of this study can serve as foundational technology in the nuclear forensics field, providing tools for the identification of signature nuclides and aiding in the research, development, comparison, and validation of related technologies.

• Journal of the Korean Society of Radiology
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• v.17 no.7
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• pp.1075-1089
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• 2023

Nuclear forensics is an essential part of nuclear material control and nuclear non-proliferation verification. Radiochronometry for nuclear forensics is used to estimate the timing of refinement and production of nuclear materials based on decay chain characteristics and the Bateman equation. The results of radiochronometry have uncertainties because the decay constant and number of nuclides are statistics derived from analyses or repeated experiments and involve uncertainties. The aim of this study was to develop an uncertainty calculation algorithm by performing computational simulation to overcome the limitations of the existing uncertainty calculation method for radiochronometry based on the Bateman equation. The results of the proposed uncertainty calculation algorithm were comparable to those of the existing method. The algorithm allowed for more than two generations of uncertainty calculations and mitigated the underestimation of the decay constant during the uncertainty calculation.

• Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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• v.20 no.2
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• pp.171-183
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• 2022

The parent and daughter nuclides in a radioactive decay chain arrive at secular equilibrium once they have a large half-life difference. The characteristics of this equilibrium state can be used to estimate the production time of nuclear materials. In this study, a mathematical model and algorithm that can be applied to radio-chronometry using the radioactive equilibrium relationship were investigated, reviewed, and implemented. A Bateman equation that can analyze the decay of radioactive materials over time was used for the mathematical model. To obtain a differential-based solution of the Bateman equation, an algebraic numerical solution approach and two different matrix exponential functions (Moral and Levy) were implemented. The obtained result was compared with those of commonly used algorithms, such as the Chebyshev rational approximation method and WISE Uranium. The experimental analysis confirmed the similarity of the results. However, the Moral method led to an increasing calculation uncertainty once there was a branching decay, so this aspect must be improved. The time period corresponding to the production of nuclear materials or nuclear activity can be estimated using the proposed algorithm when uranium or its daughter nuclides are included in the target materials for nuclear forensics.

• Journal of the Korean Society of Radiology
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• v.15 no.1
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• pp.37-43
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• 2021

Republic of Korea has many nuclear facilities in the country, and Democratic People's Republic of Korea(North Korea) locates in the surrounding country. Therefore, it is necessary to construct the target facility's nuclear forensic data in a preemptive response to the changing international situation. For this reason, this study suggests "signature" materials used to understand the origins and sources of nuclear and other radioactive materials, taking into account domestic nuclear facilities and the nuclear fuel cycle. In domestic, pressurized light water reactors and pressurized heavy water reactors are in operation, and enriched and natural uranium are used as fuels. In the front-end fuel cycle, the signature materials can be nature uranium and UF6 in the uranium enrichment process. The domestic back-end fuel cycle adopts a non-circulating cycle excluding the reprocessing process, and the primary signature material is spent nuclear fuel. According to IAEA recommendation, the importance of these materials as the signature and characteristic contents are suggested in this study. To prove the integrity of nuclear material and build a national nuclear forensics library, it is necessary to grasp the signature material and acquire the characteristic data considering the domestic nuclear facilities and the nuclear fuel cycle.

• Nuclear Engineering and Technology
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• v.47 no.5
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• pp.596-607
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• 2015

In this paper, we describe a computer program, iBEST (inverse Burnup ESTimator), that we developed to accurately estimate the burnup histories of spent nuclear fuels based on sample measurement data. The burnup history parameters include initial uranium enrichment, burnup, cooling time after discharge from reactor, and reactor type. The program uses algebraic equations derived using the simplified burnup chains of major actinides for initial estimations of burnup and uranium enrichment, and it uses the ORIGEN-S code to correct its initial estimations for improved accuracy. In addition, we newly developed a stable bisection method coupled with ORIGEN-S to correct burnup and enrichment values and implemented it in iBEST in order to fully take advantage of the new capabilities of ORIGEN-S for improving accuracy. The iBEST program was tested using several problems for verification and well-known realistic problems with measurement data from spent fuel samples from the Mihama-3 reactor for validation. The test results show that iBEST accurately estimates the burnup history parameters for the test problems and gives an acceptable level of accuracy for the realistic Mihama-3 problems.