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At least 73 records · Page 4

Evaluating Nuclear Forensic Signatures for Advanced Reactor Deployment: A Research Priority Assessment

The development and deployment of a new generation of nuclear reactors necessitates a thorough evaluation of techniques used to characterize nuclear materials for nuclear forensic applications. Advanced fuels proposed for use in these reactors present both challenges and opportunities for the nuclear forensic field. Many efforts in pre-detonation nuclear forensics are currently focused on the analysis of uranium oxides, uranium ore concentrates, and fuel pellets since these materials have historically been found outside of regulatory control. The increasing use of TRISO particles, metal fuels, molten fuel salts, and novel ceramic fuels will require an expansion of the current nuclear forensic suite of signatures to accommodate the different physical dimensions, chemical compositions, and material properties of these advanced fuel forms. In this work, a semi-quantitative priority scoring system is introduced to identify the order in which the nuclear forensics community should pursue research and development on material signatures for advanced reactor designs. This scoring system was applied to propose the following priority ranking of six major advanced reactor categories: (1) molten salt reactor (MSR), (2) liquid metal-cooled reactor (LMR), (3) very-high-temperature reactor (VHTR), (4) fluoride-salt-cooled high-temperature reactor (FHR), (5) gas-cooled fast reactor (GFR), and (6) supercritical water-cooled reactor (SWCR).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Recent Advances in Nuclear Forensic Chemistry

Nuclear forensics is a rapidly growing field with a widespread impact on global nonproliferation. From the beginning, nuclear forensic capabilities have been inextricably bound to existing limitations within chemistry and materials science. As nuclear forensics has continued to develop as a unique field of research, new advances in chemistry have revolutionized our ability to rapidly and quantitatively analyze radioactive materials for attribution. In particular, microanalytical techniques originally developed for nanoscience, such as micro-XRF, SIMS, and SEM-EDX, have enabled spatially resolved chemical analyses to be performed with only nanograms of material. Such techniques have redefined the paradigm for pre- and postdetonation nuclear forensics, as large quantities of material are no longer necessary for full characterization and attribution. This Review explains how modern nuclear forensic techniques have developed from their origins in chemistry and provides real-world examples of how these techniques have been used to characterize radioactive materials, including fallout from nuclear detonations such as the 1945 Trinity test.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Keeping the Momentum and Nuclear Forensics at Los Alamos National Laboratory

LANL has 70 years of experience in nuclear forensics and supports the community through a wide variety of efforts and leveraged capabilities: Expanding the understanding of nuclear forensics, providing training on nuclear forensics methods, and developing bilateral relationships to expand our understanding of nuclear forensic science. LANL remains highly supportive of several key organizations tasked with carrying forth the Nuclear Security Summit messages: IAEA, GICNT, and INTERPOL. Analytical chemistry measurements on plutonium and uranium matrices are critical to numerous programs including safeguards accountancy verification measurements. Los Alamos National Laboratory operates capable actinide analytical chemistry and material science laboratories suitable for nuclear material and environmental forensic characterization. Los Alamos National Laboratory uses numerous means to validate and independently verify that measurement data quality objectives are met. Numerous LANL nuclear facilities support the nuclear material handling, preparation, and analysis capabilities necessary to evaluate samples containing nearly any mass of an actinide (attogram to kilogram levels).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nuclear Forensics: Scientific Analysis Supporting Law Enforcement and Nuclear Security Investigations

In Nuclear Forensic Science, analytical chemists join forces with nuclear physicists, material scientists, radiochemists, and traditional forensic scientists, as well as experts in nuclear security, nuclear safeguards, law enforcement, and policy development, in an effort to deter nuclear smuggling. Nuclear forensic science, or “nuclear forensics,” aims to answer questions about nuclear material found outside of regulatory control, questions such as ‘where did this material come from?’ and ‘what is the intended use of the material?’ In this Feature, we provide a general overview of nuclear forensics, selecting examples of key “nuclear forensic signatures” which have allowed investigators to determine the identity of unknown nuclear material in real investigations.

07 ISOTOPE AND RADIATION SOURCES↗

Radiation History of Fission Gamma-Ray Spectra Relevant to Post-Detonation Debris Analysis

Quantifying the fissile content within trace amounts of nuclear material is of significant importance to safeguards and nuclear forensics communities. Traditionally, measurement methods have relied on destructive analysis (DA) measurements or passive detection of gamma/neutron signatures through nondestructive assay (NDA). These methods are highly accurate and employed globally as both a nuclear forensics capability and a material accountability measurement. However, common DA techniques rely on sample dissolution, a time-consuming process which can be particularly difficult for certain sample matrices, such as melt-glass formed from nuclear fallout. Likewise, trace quantities of nuclear materials prove difficult to measure using passive NDA techniques due to relatively low emission rates and potential interference from activated materials within the sample matrix.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Production of National Nuclear Material Archive Subsamples for High Precision Chemical Analysis

With its historical mission as the focal point for production of uranium components for the NNSA nuclear weapons program, the National Nuclear Materials Archive (NNMA) makes use of Y-12's wide range of uranium materials processing knowledge and onsite materials to identify, collect, and preserve sample materials for nuclear forensics purposes. In 2019, Y-12 took on the responsibility for identifying, subsampling, and shipping a total of 24 NNMA samples to the Lawrence Livermore National Laboratory (LLNL) for further forensics analysis. These were highly enriched uranium metal pieces representative of different weapon systems components produced by Y-12 from approximately 1963 to 1993. The purpose was to provide the NNMA program with higher precision analyses of these materials than what is currently available from historical Y-12 production stream data.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Policy and Technical Issues Facing a Fissile Material (Cutoff) Treaty. Chapter 14

We report the largest obstacle to creating nuclear weapons, starting with the ones that destroyed Hiroshima and Nagasaki, has been to make sufficient quantities of fissile materials – highly enriched uranium (HEU) and plutonium – to sustain an explosive fission chain reaction.1 Recognition of this fact has, for more than fifty years, underpinned both the support for and the opposition to adoption of an international treaty banning at a minimum the production of more fissile materials for nuclear weapons, commonly referred to as a fissile material cutoff treaty (FMCT).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Optical Spectroscopy Capabilities:Application to Nuclear Forensics, Nuclear Detection, Nuclear Safeguards, Oil Industry, Material Identification and Analysis, and Sustainable Agricultural Nutrient Analysis

We have been very successful in measuring and analyzing actinides and actinide containing material for concentration ranges as low as 100 ppm to metal alloys. Several publications and LA-UR spectral line assignment references have been generated from this effort and listed below (1-6).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New Routes for the Production of Fission Products and Their Separation from the Source Material for the Development of Realistic Nuclear Forensic Debris

In order to fully characterize the NIF neutron spectrum, SAND-II-SNL software was requested/received from the Radiation Safety Information Computational Center. The software is designed to determine the neutron energy spectrum through analysis of experimental activation data. However, given that the source code was developed in Sparcstation 10, it is not compatible with current version of FORTRAN. Accounts have been established through the Lawrence Livermore National Laboratory’s High Performance Computing in order to access different compiles for FORTRAN (e.g. pgf77, pgf90). Additionally, several of the subroutines included in the SAND-II-SNL package have required debugging efforts to allow for proper compiling of the code.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development of a Course in Gamma Ray Spectrometry

The majority of undergraduate and graduate students in nuclear science and engineering take a general course in nuclear instrumentation where one of the topics is typically in gamma ray spectrometry. Rarely are courses offered solely on this subject matter other than intensified workshops conducted by the International Atomic Energy Agency (IAEA) or private companies which can be expensive especially for large groups of students. Currently there are many world-wide projects in routine monitoring and advanced research that employ gamma rays. Some but not an exhaustive list of these topics include neutron activation analysis, naturally occurring radioactivity materials (NORM), nuclear forensics, nuclear security, in-situ gamma ray detection, galactic gamma ray detection, health physics and advanced instrumentation. At the Nuclear Engineering Teaching Laboratory at the University of Texas at Austin, many of our students are involved in an array of research topics that involve gamma ray spectrometry in their Masters of Science theses, PhD dissertations and special topics courses. It was decided to invest the time and effort to develop a course with a strong technical component to complement their research activities. A detailed stand-alone course in gamma ray spectrometry that includes a series lectures in modular form has been developed. As well we have incorporated fourteen advanced animations to better explain some of the fundamental physical processes and experimental set-ups. Six laboratory sessions and multiple homework assignments have also been established. This course is applicable to senior undergraduate students, graduate students, and novice researchers the above mentioned fields in a traditional class/laboratory setting or for intense one to two week workshops. A great deal of effort was undertaken to prepare a stand-alone course in gamma ray spectrometry which includes many of the fundamental aspects as well as the more advanced instrumentation. Animations of gamma ray interactions and experimental set ups were also developed. Six laboratories and six assignments were also conceived. Every topic has its own module thus a 'pick and choose' subset of lectures can be given to different levels of understanding. This course is applicable to senior undergraduate students, graduate students, novice researchers in neutron activation analysis and naturally occurring radioactive material, and for intense one to two week workshops. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fractographic Analysis of HfB2-SiC and ZrB2-SiC Composites

Hafnium diboride-silicon carbide and zirconium diboride-silicon carbide composites are potential materials for high temperature leading edge applications on reusable launch vehicles. In order to establish material constants necessary for evaluation of in-situ fracture, bars fractured in four point flexure were examined using fractographic principles. The fracture toughness was determined from measurements of the critical crack sizes and the strength values, and the crack branching constants were established to use in forensic fractography of materials for future flight applications. The fracture toughnesses range from about 13 MPam (sup 1/2) at room temperature to about 6 MPam (sup 1/2) at 1400 C for ZrB2-SiC composites and from about 11 MPam (sup 1/2) at room temperature to about 4 MPam (sup 1/2) at 1400 C for HfB2-SiC composites.

Mecholsky, J.J., Jr.↗

Electric Potential and Electric Field Imaging with Dynamic Applications & Extensions

The technology and methods for remote quantitative imaging of electrostatic potentials and electrostatic fields in and around objects and in free space is presented. Electric field imaging (EFI) technology may be applied to characterize intrinsic or existing electric potentials and electric fields, or an externally generated electrostatic field made be used for volumes to be inspected with EFI. The baseline sensor technology (e-Sensor) and its construction, optional electric field generation (quasi-static generator), and current e- Sensor enhancements (ephemeral e-Sensor) are discussed. Critical design elements of current linear and real-time two-dimensional (2D) measurement systems are highlighted, and the development of a three dimensional (3D) EFI system is presented. Demonstrations for structural, electronic, human, and memory applications are shown. Recent work demonstrates that phonons may be used to create and annihilate electric dipoles within structures. Phonon induced dipoles are ephemeral and their polarization, strength, and location may be quantitatively characterized by EFI providing a new subsurface Phonon-EFI imaging technology. Results from real-time imaging of combustion and ion flow, and their measurement complications, will be discussed. Extensions to environment, Space and subterranean applications will be presented, and initial results for quantitative characterizing material properties are shown. A wearable EFI system has been developed by using fundamental EFI concepts. These new EFI capabilities are demonstrated to characterize electric charge distribution creating a new field of study embracing areas of interest including electrostatic discharge (ESD) mitigation, manufacturing quality control, crime scene forensics, design and materials selection for advanced sensors, combustion science, on-orbit space potential, container inspection, remote characterization of electronic circuits and level of activation, dielectric morphology of structures, tether integrity, organic molecular memory, atmospheric science, weather prediction, earth quake prediction, and medical diagnostic and treatment efficacy applications such as cardiac polarization wave propagation and electromyography imaging.

Generazio, Ed↗

Codename: Audacious Aardvark

In mid-August, nine members of the Federal Bureau of Investigation (FBI) joined nine LANL employees for a three-day cross-training drill in which FBI forensics experts would train fissile material handlers in the work of traditional forensics on nuclear components. The drill was called Audacious Aardvark, reflecting an aardvark’s diligence and fearlessness.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Reconstruction and Failure Analysis of the Space Shuttle Columbia

Several days following the Columbia accident a team formed and began planning for the reconstruction of Columbia. A hangar at the Kennedy Space Center was selected for this effort due to it's size, available technical workforce and materials science laboratories and access to the vehicle ground processing infrastructure. The Reconstruction team established processes for receiving, handling, decontamination, tracking, identifying, cleaning and assessment of the debris. Initially, a 2-dimensional reconstruction of the Orbiter outer mold line was developed. As the investigation progressed fixtures which allowed a 3-dimensional reconstruction of the forward portions of the left wing's leading edge was developed. To support the reconstructions and forensic analyses a Materials and Processes (M&P) 'team was formed. This M&P team established processes for recording factual observations, debris cleaning, and engineering analysis. Fracture surfaces and thermal effects of selected airframe debris were assessed, and process flows for both nondestructive and destructive sampling and evaluation of debris were developed. The Team also assessed left hand airframe components that were believed to be associated with a structural breach of Columbia. A major portion of this analysis was evaluation of metallic deposits were prevalent on left wing leading edge components. Extensive evaluation of the visual, metallurgical and chemical nature of the deposits provided conclusions that were consistent with the visual assessments and interpretations of the NASA lead teams and the findings of the Columbia Accident Investigation Board. Analytical data collected by the M&P Team showed that a significant thermal event occurred at the left wing leading edge in the proximity of LH RCC Panels 8-9, and a correlation was formed between the deposits and overheating in these areas to the wing leading edge components. The analysis of deposits also showed exposure to temperatures in excess of 1649 C (3200 F), which would severely degrade support structure, tiles, and RCC panel materials. The integrated failure analysis of wing leading edge debris and deposits strongly supported the hypothesis that a breach occurred at LH RCC Panel 8.

Russell, Richard↗

In-situ Synthesis of PuCl 3 and Corresponding Raman and Density Functional Theory Vibrational Modes

The experimental and calculated Raman spectrum of PuCl 3 has been reported for the first time. PuCl 3 is a primary species found in plutonium metal refinement, specifically in pyrochemical salt processes including multicycle direct oxide reduction, metal chlorination, and electrorefining. As such, Raman signatures of PuCl 3 could serve as potential forensic indicators of material process history. A novel technique for synthesizing PuCl 3 from the in situ chlorination of plutonium metal with HCl was developed to establish these signatures. Cerium metal surrogates were utilized to ensure optimization of the plutonium experiments and to minimize personnel exposure, and all experiments were carried out in a Raman reaction chamber designed for air-tight, high vacuum environments. In situ Raman spectroscopy was employed in conjunction with density functional theory (DFT) to investigate the vibrational modes of PuCl 3 . Associated mixed oxy and hydroxyl phases are also reported. The combined Raman and DFT results have eliminated inconsistencies in Raman mode assignments for the MX 3 family of metal chlorides having P6 3 /m symmetry, and IR modes derived from the DFT calculations are additionally presented. The data observed in this study are of potential interest to nuclear forensic analyses, nuclear sample aging, nuclear energy, plutonium processing, and stockpile stewardship.

36 MATERIALS SCIENCE↗