Characterization Of Nuclear Materials Research Articles

A Monte Carlo simulation code for calculating damage and particle transport in solids: The case for electron-bombarded solids for electron energies up to 900 MeV

Current popular Monte Carlo simulation codes for simulating electron bombardment in solids focus primarily on electron trajectories, instead of electron-induced displacements. Here we report a Monte Carol simulation code, DEEPER (damage creation and particle transport in matter), developed for calculating 3-D distributions of displacements produced by electrons of incident energies up to 900 MeV. Electron elastic scattering is calculated by using full-Mott cross sections for high accuracy, and primary-knock-on-atoms (PKAs)-induced damage cascades are modeled using ZBL potential. We compare and show large differences in 3-D distributions of displacements and electrons in electron-irradiated Fe. The distributions of total displacements are similar to that of PKAs at low electron energies. But they are substantially different for higher energy electrons due to the shifting of PKA energy spectra towards higher energies. The study is important to evaluate electron-induced radiation damage, for the applications using high flux electron beams to intentionally introduce defects and using an electron analysis beam for microstructural characterization of nuclear materials.

Lock-in thermography for characterization of nuclear materials

A simplified procedure of lock-in thermography was developed and applied for characterization of nuclear materials. The possibility of thickness and thermal diffusivity measurements with the accuracy better than 90% was demonstrated with different metals and Zircaloy-4 claddings.

Laser driven nuclear science and applications: The need of high efficiency, high power and high repetition rate Laser beams

Extreme Light Infrastructure (ELI) is a pan European research initiative selected on the European Strategy Forum on Research Infrastructures Roadmap that aims to close the gap between the existing laboratory-based laser driven research and international facility-grade research centre. The ELI-NP facility, one of the three ELI pillars under construction, placed in Romania and to be operational in 2018, has as core elements a couple of new generation 10 PW laser systems and a narrow bandwidth Compton backscattering gamma source with photon energies up to 19 MeV. ELI-NP will address nuclear photonics, nuclear astrophysics and quantum electrodynamics involving extreme photon fields. Prospective applications of high power laser in nuclear astrophysics, accelerator physics, in particular towards future Accelerator Driven System, as well as in nuclear photonics, for detection and characterization of nuclear material, and for nuclear medicine, will be discussed. Key issues in these research areas will be at reach with significant increase of the repetition rates and of the efficiency at the plug of the high power laser systems as proposed by the ICAN collaboration.

Neutron- and X-ray radiography/ tomography: non-destructive analytical tools for the characterization of nuclear materials

Neutron- and X-ray radiography/ tomography: non-destructive analytical tools for the characterization of nuclear materials

Application of Wavelet Unfolding Technique in Neutron Spectroscopic Analysis

Nonproliferation of nuclear materials is important in nuclear power industry and fuel cycle facilities. It requires technologies capable of measuring and assessing the radiation signatures of fission events. Neutrons produced in spontaneous or induced fission reactions are mainly fast. The neutron energy information allows characterization of nuclear materials and neutron sources. It can also be applied in remote sensing and source search tasks. The plastic scintillator EJ-299-33A was studied as a fast neutron detector. The detector response to a polyenergetic flux was unfolded usingthe multiple linear regression method. It yields the intensities of neutron flux of particular energy, hence, enabling the spectroscopic analysis. The wavelet technique was evaluated for the unfolding of neutron spectrum using the scintillator's response functions between 1 MeV and 14 MeV computed with the MCNPX code. This paperpresents the computational results of the wavelet-based spectrum unfolding applied to a scintillator detector with neutron / photon pulse shape discrimination properties.

Advanced x-ray spectrometric techniques for characterization of nuclear materials: An overview of recent laboratory activities

Advancements in x-ray spectrometric techniques at different stages have made this technique suitable for characterization of nuclear materials with respect to trace/major element determinations and compositional uniformity studies. The two important features of total reflection x-ray fluorescence spectrometry: 1) requirement of very small amount of sample in ng level 2) multielement analytical capability, in addition to other features, make this technique very much suitable to nuclear materials characterization as most of the nuclear materials are radioactive and the radioactive waste generated and radiation hazards to the operator are minimum when such low amount of sample is used. Similarly advanced features of energy dispersive x-ray fluorescence e.g. better geometry for high flux, reduction in background due to application of radiation filters have made the measurements of samples sealed inside thin alkathene/PVC covers possible with good sensitivity. This approach avoids putting the instrument inside a glove box for measuring radioactive samples and makes the operation/maintenance of the instrument and analysis of the samples possible in easy and fast manner. This approach has been used for major element determinations in mixed uranium–plutonium samples. Similarly μ-XRF with brilliant and micro-focused excitation sources can be used for compositional uniformity study of reactor fuel pellets. A μ-XRF study using synchrotron light source has been made to assess the compositional uniformity of mixed uranium–thorium oxide pellets produced by different processes. This approach is simple as it does not involve any sample preparation and is non-destructive. A brief summary of such activities carried out in our laboratory in past as well as ongoing and planned for the future have been discussed in the present manuscript.

Characterization of Nuclear Materials in Extreme Conditions: Raman Spectroscopy Approach

A review is given of our last advances on Raman spectroscopy characterization of irradiated and/or leached UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> , PuO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> and (U,Pu)O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> samples. For this purpose, three original Raman setups dedicated to the study of nuclear materials were involved. In every case, irradiation-induced Raman defect bands in the 500 - 750 cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-1</sup> range was observed. For UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> , an annealing temperature experiment suggests that these defect bands could be the signatures of medium-range structured defects. Besides, the leaching experiments show different behavior between the irradiated in situ probed UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> ceramic and post mortem probed [UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> + (U,Pu)O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> ] sample: The growth of an altered layer made of studtite and schoepite phases was monitored at the surface of UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> ceramic, while post-mortem studies reveal the presence of U <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">8</sub> and studtite phases at the surface of the UO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> grains of the binary sample. No alteration layer was observed at the surface of the leached (U,Pu)O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> grains.

Characterization of nuclear materials by total reflection X-ray fluorescence spectrometry

Nuclear energy is one of the available energy options for long term energy security of world. In order to produce electricity using this mode of energy generation in an efficient and safe manner, it is necessary that the materials used for such energy generation comply with the specifications assigned. The major and trace composition of these materials is an important specification for their quality control. Different analytical techniques are used for such quality control. Total reflection X-ray fluorescence (TXRF) is a comparatively new technique having several features well suited for trace and major element determinations in nuclear materials. However, this technique has not been used so far extensively for characterization of nuclear materials. The present paper gives a brief introduction of TXRF, its suitability for nuclear material characterization and some details of the TXRF studies made in our laboratory for the characterization of nuclear materials.

Application of micro-XRF for nuclear materials characterization and problem solving

A number of spatially resolved elemental imaging techniques are commonly employed to examine plutonium and other nuclear materials (e.g., scanning electron microscopy). Up until the past 10–15 years, micro-X-ray fluorescence (MXRF) instrumentation had been relatively uncommon, and even currently, it is underutilized for spatially resolved nuclear materials analysis and imaging. In the current study, a number of plutonium materials problem solving applications are presented to demonstrate the power and utility of MXRF for providing unique, spatially resolved elemental composition information. Applications discussed include identification of multiple insoluble fractions in plutonium and neptunium mixed oxide, spatially resolved imaging of plutonium residue and other elements on surface swipes, and spatial mapping of impurities in plutonium metal. The mixed oxide particle analysis demonstrated the ability to non-destructively identify particles of interest for potential extraction and analysis by other methods. The surface swipes study demonstrated the unique ability of MXRF to non-destructively image large multiple cm2 sized, non-conducting, radiologically contaminated samples. The plutonium metal investigation showed the capability of MXRF to non-destructively map elemental heterogeneity directly in an actinide matrix. Such information is extremely valuable prior to using destructive analysis (DA) trace elemental analytical chemistry techniques. If a metal is found to contain significant elemental impurity heterogeneity by MXRF, time consuming destructive sample preparation and analysis do not need to be repeated to confirm that the sample is indeed heterogeneous.

Nuclear Materials Characterization by Tomographic Atom Probe

Nuclear Materials Characterization by Tomographic Atom Probe

Measurement of boron isotopic ratio with non-gated molecular spectroscopy of femtosecond laser-produced plasma

Laser-induced breakdown spectroscopy can be augmented by concurrent spectroscopic measurements of molecules and molecular ions resulting from recombination of laser-ablated plasmas with the ablated sample and surrounding environment. Molecular emissions can exhibit significantly greater isotopic shifts than atomic emissions, making this approach attractive for isotopic characterization of nuclear materials. We describe a measurement of boron isotopic ratios in four boron-containing samples utilizing the emission from boron monoxide radicals formed in the expanding laser-induced ablation plume. Femtosecond laser excitation is used and the emission in the 532–540nm region of interest is studied, where a linear superposition of characteristic spectra for two boron isotopes has been applied for reconstruction of the boron isotopic ratio. It is also demonstrated that the use of non-gated measurements of emission spectra suffices for accurate isotopic characterization using this method. The application of multivariate regression to deconvolve the isotopic ratio from the measured emission spectra is discussed in detail, including the limitations and subtleties of this approach.

Total reflection X-ray fluorescence and energy-dispersive X-ray fluorescence characterizations of nuclear materials

Nuclear energy is one of the clean options of electricity generation for the betterment of human life. India has an ambitious program for such electricity generation using different types of nuclear reactors. The safe and efficient generation of electricity from these reactors requires quality control of different nuclear materials, e.g. nuclear fuel, structural materials, coolant, moderators etc. These nuclear materials have to undergo strict quality control and should have different specified parameters for their use in nuclear reactors. The concentration of major and trace elements present in these materials should be within specified limits. For such chemical quality control of these materials, major and trace elemental analytical techniques are required. Since some of these materials are radioactive, the ideal chemical characterization techniques should have multielement analytical capability, should require very less sample (micrograms level) for analysis so that the radioactive waste generated, and radiation exposure to the detector and operator are minimum. Total reflection X-ray fluorescence (TXRF) and energy dispersive X-ray fluorescence (EDXRF) with improved features, e.g. application of filters, secondary target and instrumental geometry require very small amount of sample and thus can be suitably used for the characterization of nuclear materials mainly for the determination of elements at trace and major concentration levels. In Fuel Chemistry Division, TXRF analytical methods have been developed for trace element determinations in uranium and thorium oxides, chlorine determination in nuclear fuel and cladding materials, sulphur in uranium, uranium in sea water etc. Similarly, EDXRF analytical methods with radiation filters (to reduce background) and improved sample preapartion techniques, e.g. fusion bead and taking samples in the form of solution on filter papers have been used for developing analytical methods for the determination of U and Th in their mixed matrices, Cd in uranium etc. Some of these studies have been reported in this paper.

Plutonium metal standards exchange program for actinide measurement quality assurance (2001–2007)

Plutonium metal exchange programs operated by the Rocky Flats Plant were conducted from 1956–1989 to ensure quality and to compare measurements in a plutonium metal matrix. Los Alamos National Laboratory (LANL) re-established the program in 2001 to assess the quality of analytical chemistry capabilities that support special nuclear material characterization. It is the only program of its kind for the preparation and distribution of plutonium metal reference materials with a range of impurity contents to multiple laboratories for destructive measurements of elemental concentration, isotopic abundance, and both metallic and non-metallic impurity levels. This program provides independent verification of analytical measurement capabilities for each of the seven currently participating laboratories, and allows any technical problems with analytical measurements to be identified and corrected. This paper focuses on basic program elements and presents a summary of methods and results for plutonium, uranium, neptunium, and americium, measurements.

Nuclear, chemical, and physical characterization of nuclear materials

The goal of nuclear forensics is to establish an unambiguous link between illicitly trafficked nuclear material and its origin. The Los Alamos National Laboratory (LANL) Nuclear Materials Signatures Program has implemented a graded “conduct of operations” type analysis flow path approach for determining the key nuclear, chemical, and physical signatures needed to identify the manufacturing process, intended use, and origin of interdicted nuclear material. This analysis flow path includes both destructive and non-destructive characterization techniques and has been exercized against different nuclear materials from LANL’s special nuclear materials archive. Results obtained from the case study will be presented to highlight analytical techniques that offer the critical attribution information.

Study of a new boron loaded plastic scintillator (revised)

Neutron detection research using plastic scintillators has recently led to instrument development for several applications and particularly for nuclear material characterization. In particular, plastic scintillators exhibit a fast time response and a high efficiency for fast neutrons spectrometry. The use of boron loaded plastic scintillators has been also proposed in order to reduce dead time for fission neutron coincidence counting. We report here on the study of a new and low-cost boron loaded plastic scintillator. Further, a simulation study was performed, including light production and transport in this kind of scintillator. Its characteristics have been measured in terms of light response, photon and neutron induced signals. An experiment has been carried out using the ion beam of a Van de Graaff accelerator at Saclay so as to determine the Birks parameters of the scintillators. These parameters were obtained for proton (between 1-2 MeV) and alpha particles (between 3.1 MeV and 5.4 MeV). The correlation between the experimental data and the simulation predictions has been studied for the neutron response of these scintillators. In addition, performances of this scintillator are compared with those of commercially available boron loaded plastic scintillator (BC454 from Bicron, Newbury, OH).

Study of a new boron loaded plastic scintillator

Neutron detection research using plastic scintillators has recently led to instrument development for several applications and particularly for nuclear material characterization. In particular, plastic scintillators exhibit a fast time response and a high efficiency for fast neutrons spectrometry. The use of boron loaded plastic scintillators has been also proposed in order to reduce dead time for fission neutron coincidence counting. We report on the study of a new and low-cost boron loaded plastic scintillator. Further, a simulation study was performed, including light production and transport in this kind of scintillator. Its characteristics have been measured in terms of light response, photon and neutron induced signals. An experiment has been carried out using the ion beam of a Van de Graaff accelerator at Saclay so as to determine the Birks parameters of the scintillators. These parameters were obtained for proton (between 1-2 MeV) and alpha particles (between 3.1 MeV and 5.4 MeV). The correlation between the experimental data and the simulation predictions has been studied for the neutron response of these scintillators. In addition, the performance of this scintillator are compared with those of a commercially available boron loaded plastic scintillator (BC454 from Bicron, Newbury, OH).

Cyclic Voltammetric Behavior of Uranyl ion in Sulfuric Acid Solutions. Application to Some Nuclear Materials Characterization

Abstract The U(VI) reduction at mercury electrode in sulfuric acid solutions was examined by cyclic voltammetry (C. V.). A diffusion coefficient, D, was (5.30 ± 0.08) × 10−6 cm2/sec was obtained for the depolarizer at 25.0±0.2°C in 1 N K2SO4 (pH = 2). In 1 N K2SO4/1 N H2,SO4 systems the disproportionation of U(V) was found to occur with the constant rate of Kd/[H+] = 6.500 ± 1.000 M−2 sec−1. In 1 M H2SO4 supporting electrolyte pure kinetic control was achieved over the range of scan rates and uranyl concentration (C) investigated, hence linear correlation between cathodic peak current and C (above 5x10−6 M) was obtained. Strong complexing oxyanions, such as phosphate and pyrosulphate, do not interfere with the cathodic peak current. Rapid determination of O/U ratios in uranium oxides and of U in mixed U-Th materials were performed respectively in 1 M H2SO4/1.5 M H3PO4 and 1 M H2SO4/0.2 M K2S204 supporting media, with a reproducibility of ± 1.3% standard deviation.