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NASA NTRS2015

Nuclear Thermal Propulsion Development Risks

There are clear advantages of development of a Nuclear Thermal Propulsion (NTP) for a crewed mission to Mars. NTP for in-space propulsion enables more ambitious space missions by providing high thrust at high specific impulse ((is) approximately 900 sec) that is 2 times the best theoretical performance possible for chemical rockets. Missions can be optimized for maximum payload capability to take more payload with reduced total mass to orbit; saving cost on reduction of the number of launch vehicles needed. Or missions can be optimized to minimize trip time significantly to reduce the deep space radiation exposure to the crew. NTR propulsion technology is a game changer for space exploration to Mars and beyond. However, 'NUCLEAR' is a word that is feared and vilified by some groups and the hostility towards development of any nuclear systems can meet great opposition by the public as well as from national leaders and people in authority. The public often associates the 'nuclear' word with weapons of mass destruction. The development NTP is at risk due to unwarranted public fears and clear honest communication of nuclear safety will be critical to the success of the development of the NTP technology. Reducing cost to NTP development is critical to its acceptance and funding. In the past, highly inflated cost estimates of a full-scale development nuclear engine due to Category I nuclear security requirements and costly regulatory requirements have put the NTP technology as a low priority. Innovative approaches utilizing low enriched uranium (LEU). Even though NTP can be a small source of radiation to the crew, NTP can facilitate significant reduction of crew exposure to solar and cosmic radiation by reducing trip times by 3-4 months. Current Human Mars Mission (HMM) trajectories with conventional propulsion systems and fuel-efficient transfer orbits exceed astronaut radiation exposure limits. Utilizing extra propellant from one additional SLS launch and available energy in the NTP fuel, HMM radiation exposure can be reduced significantly.

Kim, Tony↗
DOE OSTI2020

Preliminary Evaluation of Driver Fuel Plates and Reduced Sodium Temperature to Increase Fast Test Reactor Experimental Neutron Irradiation Capabilities

All sodium-cooled fast test reactors operated so far have used essentially the same fuel geometrical ar-rangement, namely cylindrical fuel pins assembled into a triangular array in hexagonal fuel assemblies. Fuel compositions and dimensions may vary but the overall geometrical pattern remains identical. Fur-thermore, most sodium-cooled reactors have operated, and still operate, with core-average inlet and outlet sodium temperatures of, respectively, 350-400°C and 500-550°C. The present preliminary study revisits the standard fuel assembly geometry as well as operating tempera-tures to evaluate potential impact on fast test reactor neutron irradiation capabilities. The reference fuel is U-20Pu-10Zr. Pin (reference) and plate geometries are considered together with two sets of core-average sodium inlet/outlet temperatures: 350/500°C (reference) and 200/400°C. More prototypic environments could be obtained inside ad-hoc irradiation testing vehicles that are independent from the reactor primary coolant. Everything else being the same, fuel temperature is significantly lower in plates than in pins. Therefore, plates could in principle accommodate higher plutonium content, thus, reducing the need for uranium enrichment or allowing the use of lower quality plutonium (U-xPu-10Zr thermal conductivity and solidus temperature decrease as x increases, hence, necessitating additional thermal margins). For the reference pin configuration, lowering the inlet/outlet sodium temperatures from the reference 350/500°C down to 200/400°C provides additional thermal margins that can be used to increase the peak fast flux from about 4.5 × 10 15 n/cm 2 -s to 6 ×10 15 n/cm 2 -s for the same core power of 300 MW. Assuming 300 Equivalent Fuel Power Days (EFPD) of operation per calendar year, a (steel) test article could accu-mulate up to 75 dpa/year. The use of fuel plates provides even more thermal margins which may allow the peak fast flux to reach values as high as 8 × 10 15 n/cm 2 -s for both sets of inlet/outlet temperatures. In this environment, a test article could accumulate up to 95 dpa/year assuming 300 EFPD/year, hence greatly accelerating irradiation testing. Allowing a fast test reactor to operate over a wide range of inlet/outlet temperatures could add significant flexibility to its neutron irradiation capabilities. Steel present in the driver fuel assemblies is not expected to accumulate more than 90 displacements per atom (dpa) over its lifetime. Hence, steel alloys that are not suited for very high dpa but can operate over a wide range of temperatures (from low to high) would be appropriate for this application. Finally, because pin and plate assemblies fit on the same grid plate, a fast test reactor could in principle start-up with standard fuel pin assemblies and, later on, move to a plate-type Mark-II fuel to further in-crease its neutron irradiation capabilities while potentially reducing the level of uranium enrichment needed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Final CRADA Report: Accelerated Burn-up Accumulation Test of Clean Core Thorium Energy Designated ANEEL Fuel

Clean Core Thorium Energy (CCTE), LLC, located in Oak Brook, Illinois, is committed to the development of alternative nuclear fuels. CCTE is focused on leveraging the inherent benefits of thorium to create a novel nuclear fuel solution for our worlds growing power demand. Unlike some other fuel cycles proposing to use thorium in advanced reactors, CCTE is focused on deploying solid fuel designs (ceramic pellets in metallic cladding) in existing pressurized heavy-water reactors (PHWRs) and Canada deuterium uranium (CANDU) reactors. CCTE’s fuel design, referred to as Advanced Nuclear Energy for Enriched Life (ANEEL), uses mixed thorium-uranium oxide ((Th,U)O2) to enhance reactor operational strategies while producing significantly low attractiveness material in terms of nuclear proliferation. The overall project objective is to investigate the performance of high burnup ANEEL fuel via an irradiation experiment to be performed in the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). The scope of work for this CRADA was specifically aimed at performing conceptual design and analysis to support development of an irradiation test rig, development of a fuel fabrication process for the experiment pellets, fabrication and qualification of the pellets, and shipment of the pellets to INL so they can be used to construct experiment rodlets.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Massachusetts Institute of Technology Reactor LEU Fuel Element Flow Test Conceptual Design – Hydraulic Reactor Design Parameters

The Massachusetts Institute of Technology Reactor (MITR-II, also referred to as MITR) is one of six U.S. high performance research reactors (USHPRR), including one critical facility, that is actively collaborating with the U.S. National Nuclear Security Administration (NNSA) Material Management and Minimization (M 3 ) Reactor Conversion Program to convert to the use of low-enriched uranium (LEU, < 20 wt% 235 U) fuel. The MIT Nuclear Reactor Laboratory has been working with the USHPRR Reactor Conversion (RC) Pillar at Argonne National Laboratory to perform fuel element design and fuel cycle performance analyses, steady-state thermal hydraulics safety analyses, and accident safety analyses in preparation for the conversion of MITR and support a preliminary Safety Analysis Report (SAR) for conversion to LEU fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Nonfuel antineutrino contributions in the ORNL High Flux Isotope Reactor (HFIR)

Reactor neutrino experiments have seen major improvements in precision in recent years. With the experimental uncertainties becoming lower than those from theory, carefully considering all sources of $\bar{ν}$ e is important when making theoretical predictions. One source of νe that is often neglected arises from the irradiation of the nonfuel materials in reactors. The $\bar{ν}$ e rates and energies from these sources vary widely based on the reactor type, configuration, and sampling stage during the reactor cycle and have to be carefully considered for each experiment independently. In this article, we present a formalism for selecting the possible $\bar{ν}$ e sources arising from the neutron captures on reactor and target materials. We apply this formalism to the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory, the $\bar{ν}$ e source for the the Precision Reactor Oscillation and Spectrum Measurement (PROSPECT) experiment. Overall, we observe that the nonfuel $\bar{ν}$ e contributions from HFIR to PROSPECT amount to 1% above the inverse beta decay threshold with a maximum contribution of 9% in the 1.8–2.0 MeV range. Nonfuel contributions can be particularly high for research reactors like HFIR because of the choice of structural and reflector material in addition to the intentional irradiation of target material for isotope production. We show that typical commercial pressurized water reactors fueled with low-enriched uranium will have significantly smaller nonfuel $\bar{ν}$ e contribution.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2025

Controlled Reaction Dynamics of Binary Hexafluorides to Explore New Chemical Signatures

Uranium hexafluoride (UF6 ) is a key compound in the nuclear fuel cycle. • Many enrichment technologies utilize UF6 due to its advantageous properties: • Fluorine (F) has only one isotope of major abundance. • UF6 is a solid at room temperature but has a high (~70 torr) vapor pressure. • There is significant knowledge regarding the chemical processing of UF6 . • UF6 readily hydrolyzes when released to the atmosphere. • Despite significant advances in UF6 processing, the fundamental chemistry governing reaction with UF6 is still poorly understood.

Dorris, Austin L. [Savannah River National Laborat↗
DOE OSTI2021

Analysis and Design for Irradiation of High Power TRISO Fuel Compact Specimens in HFIR

Tristructural isotropic (TRISO) fuel is being proposed for use in several high-temperature advanced reactor concepts because of its structural integrity under high operating temperatures and burnup. One of these advanced reactor concepts is the Kairos Power fluoride salt-cooled high-temperature reactor (KP- FHR) under development by Kairos Power, LLC. Previous TRISO irradiation experiments were focused on qualification for high-temperature gas reactors (HTGRs), which have higher operating temperatures but lower particle powers than the KP-FHR design. To study the performance of TRISO fuel designed for HTGRs under prototypical FHR conditions, a set of experiments was designed using the MiniFuel irradiation vehicle at the Oak Ridge National Laboratory’s (ORNL) High Flux Isotope Reactor (HFIR). The experiments will irradiate 30 TRISO-containing carbon matrix compacts at inner small vertical experiment facilities in HFIR. Each compact will contain 20 TRISO particles (600 particles total) developed for HTGRs, consisting of either 14% enriched uranium dioxide uranium carbide, naturally enriched uranium dioxide, uranium carbide, or 9.6% enriched uranium dioxide fuel kernels with time- and volume-averaged silicon carbide layer temperatures between 500 and 900°C. This report summarizes the vehicle designs that have been developed, as well as the neutronic and thermal analyses completed for these irradiation experiments. These analyses show that MiniFuel compact irradiation is a versatile experiment that can be used to study a range of TRISO particle powers and fuel types while providing reasonable separation of burnup and temperature effects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS2022

Lattice Confinement Fusion and Fusion-Fast-Fission Energy Source Development

NASA and the US Navy have demonstrated Lattice Confinement Fusion (LCF) and the Fusion-Fast-Fission of natural uranium and thorium. Both methods build upon decades of research, and the latter benefits from conventional nuclear fission and fusion results. However, this nascent technology doesn’t require fissile isotopes and avoids nuclear weapons proliferation concerns from uranium 235U isotopic enrichment or plutonium 239Pu separation. Of particular note, LCF doesn’t need power hungry magnets, lasers, or particle beams. Potentially, it could provide watts to hundreds of kilowatts of electrical power and process heat suitable for space power and high Isp nuclear electric propulsion (NEP) as well as distributed terrestrial power. Finally, there are indications that LCF fast-fission products are more benign than those of conventional fission reactors. Our goal is to scale the reactions and increase the power output through higher temperature operation and increased material masses.

lattice confinement fusion↗
DOE OSTI2023

Plutonium Signatures in Molten-Salt Reactor Off-Gas Tank and Safeguards Considerations

Fluid-fueled molten-salt reactors (MSRs) are actively being developed by several companies, with plans to deploy them internationally. The current IAEA inspection tools are largely incompatible with the unique design features of liquid fuel MSRs (e.g., the complex fuel chemistry, circulating fuel inventory, bulk accountancy, and high radiation environment). For these reasons, safeguards for MSRs are seen as challenging and require the development of new techniques. This paper proposes one such technique through the observation of the reactor’s off-gas. Any reactor design using low-enriched uranium will build up plutonium as the fuel undergoes burnup. Plutonium has different fission product yields than uranium. Therefore, a shift in fission product production is expected with fuel evolution. The passive removal of certain gaseous fission products to the off-gas tank of an MSR provides a valuable opportunity for analysis without significant modifications to the design of the system. Uniquely, due to the gaseous nature of the isotopes, beta particle emissions are available for observation. The ratios of these fission product isotopes can, thus, be traced back to the relative amount and types of fissile isotopes in the core. This proposed technique represents an effective safeguards tool for bulk accountancy which, while avoiding being onerous, could be used in concert with other techniques to meet the IAEA’s timeliness goals for the detection of a diversion.

Dunkle, Nicholas (ORCID:000000027323011X)↗
DOE OSTI2020

Gamma ray Imaging Based Methods to Improve the Accuracy of Uranium Holdup Quantification

Deposits in commercial uranium processing facilities of interest to nuclear safeguards are predominantly low enriched uranium (LEU). The shapes and sizes of holdup deposits can vary significantly, thus making it difficult to model the deposits accurately for calibration purposes. This presents a challenge to currently employed methods such as the Generalized Geometry Holdup (GGH) that rely on quantifying 235U mass by simplifying deposit shapes as a point, a line, or an area. In this work, gamma ray imaging using high energy resolution Germanium Gamma Imagers (GeGI™) is employed to determine the distribution of uranium inside the source containment. Two types of imaging methods are employed; coded-aperture imaging and Compton imaging. Gamma-ray emissions seen in different regions of the image are quantified using an inverse gamma-ray transport solver being developed at ORNL. Using measured data, the inverse method will be used to solve for unknown source parameters such as source matrix thickness, density, and attenuation due to container wall and shielding. The intrinsic efficiency of the detector is determined based on a library of built-in response functions and key dimensions of the detector (e.g., thickness and radius of the detector crystal). Measurements are performed in both imaging modalities using uranium sources of well-known masses and enrichments configured inside mocked-up holdup fixtures. Results from the two imaging modalities are intercompared. The paper presents preliminary results of the imaging measurements and the progress made in the computational methods to quantify uranium mass.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2023

Volume 9: Critical Facility with Add-On Ion Beam

Completion of the originally planned critical facility has been considered as part of the High Flux Isotope Reactor (HFIR) Sustaining and Enhancing Neutron Science Initiative at Oak Ridge National Laboratory (ORNL). A working group of ORNL staff members was formed to develop the idea and to recommend one or more configurations to best support future HFIR operations and scientific capacities. HFIR was designed with a critical pool in the reactor bay that was projected to be outfitted as a critical facility. The primary purpose of the planned critical facility was to measure the subcritical worth of fresh fuel elements to support startup requirements. However, the Y-12 National Security Complex already housed a critical facility that was used for this purpose. This report presents the working group’s efforts, including determination of the proposed critical facility’s high-impact benefits. A generic low-power critical facility would be employed for reactor physics measurements, code and data validation, reactor operator and staff training, and education. This facility would be instrumental in supporting current HFIR operations, conversion of HFIR to low-enriched uranium, existing light water reactor operations, and advanced reactor development and deployment.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRSDate not supplied

Molten Salt Lattice Confinement Fusion (LCF) Fast Fission Reactor for Lunar and Planetary Surface Power

Molten salt fission reactors (MSR) have been suggested for lunar and planetary surface power systems. They have the advantage of operating at high temperature, for efficient thermal-electrical conversion, low pressure, long-lived with high nuclear fuel burnup. MSR are often designed to breed fissile 233U from natural 232Th by neutron capture and  decay via: 232Th(n,)233Th(,)233Pa(,)233U Unfortunately, this process requires 233Pa isotope separation and segregation to decay to 233U. This requirement prevents additional neutron capture that interferes with 233U breeding. Instead, Wooley’s sub-critical, fast fission, molten salt reactor would use externally generated tokamak fusion neutrons1,2 to fission all actinides.We propose a simpler fusion-fast-fission sub-critical reactor that generates fast neutrons in situ from lattice confinement fusion (LCF) to fission fertile and fissile actinides. This hybrid reactor doesn't require enriched 235U fissile pins to initiate fis-sion reactions, nor 233Pa separation and segregation during operation. Like Wooley’s, this hybrid reactor “burns” natural uranium (238U) or thorium (232Th) which avoids uranium enrichment and additional fissile material launch safety and security costs. The LCF neutron source is initiated by bremsstrahlung photoneutrons (Fig. 1)3 or isotopic neutron sources in electron-screened lattices (Fig. 2)4,5. Alternatively, the electrolytic Pd-deuterium co-deposition6protocol fast fissions7 both 232Th and 238U. However, an aqueous electrolyte-based system, without pressurization similar to conventional pressurized water fission reactors, is incapable of high temperatures due to the boiling point of the electrolyte slightly over 100 C. Molten salts can be used instead as was demonstrated at the University of Hawaii8 using a variety of Ni and Pd cathodes in lithiated, hydrided and deuterated salts. These salts have melting points often exceeding 500C making them suitable to efficiently produce electrical power9 through either Advanced Stirling Genera-tors (< 100 kWe) or closed-Brayton Cycle (> 100 kWe). This hybrid reactor could power a wide range of lunar or Martian applications from unmanned in-struments, to charging vehicles and entire facilities such as human habitats or in situ resource utilization. The power conversion cycles are Carnot Cycle limited, but generally 30% efficient at best. However, waste heat on the moon or Mars is important to surviving either two-week lunar nights or Martian nights as well as providing process heat for mineral extraction and “living off the land”

Lawrence Forsley↗
DOE OSTI2022

Bioinspired Macrocyclic Molecule Supported Two‐Dimensional Lamellar Membrane with Robust Interlayer Structure for High‐Efficiency Nanofiltration

Abstract 2D lamellar membranes (2DLMs) are used for efficient desalination and nanofiltration. However, weak interactions between adjacent stacked nanosheets result in susceptibility to swelling that limits practical applicability. Inspired by the super adhesion of multi‐point suction cups on octopus tentacles, a 2DLM is constructed from Ti 3 C 2 T x MXene supported by the macrocyclic “multi‐point” molecule cucurbit[5]uril (CB5) and demonstrated for nanofiltration of methyl blue (MB) and enrichment of uranyl carbonate. Experimental results and density functional theory calculations indicate that CB5 rivets to the surface of the nanoflakes through strong stable interactions between its multiple binding sites and surface hydroxyl functional groups on MXene nanosheets. This novel 2DLM exhibits excellent nanofiltration performance (69 L m −2 h −1 bar −1 permeance with 93.6% rejection for MB) and can be recycled at least 30 times without significant degradation. The 2DLM exhibits excellent swelling resistance at high salinity, with a demonstration of selective enrichment of uranyl carbonate from artificial water and natural seawater. The results provide a new strategy for constructing highly stable 2DLMs with interlayer spacing controllable from sub‐nano to nanometer scales, for size‐selective sieving of molecules and ions, high‐efficiency nanofiltration, and other applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Technical Evaluation of Accelerated Basin De-Inventory Material Addition to Sludge Batch 11

Savannah River Nuclear Solutions has a need to discard spent nuclear fuel (SNF), currently stored in L Basin, to the Defense Waste Processing Facility (DWPF) for vitrification. The Department of Energy (DOE) has approved the Accelerated Basin De-inventory (ABD) Program for discarding SNF via transfers from H-Canyon to the Savannah River Site (SRS) Liquid Waste (LW) system. The first ABD discards will occur during the preparation of Sludge Batch (SB) 11. An initial impact evaluation of the LW flowsheet was performed by the Savannah River National Laboratory (SRNL) prior to the approval of the ABD Program. This evaluation addressed the LW downstream facilities based on the current H-Canyon flowsheet sequence for the average ABD discard. The flowsheet evaluation only included aluminum-clad SNF, specifically Materials Test Reactor (MTR) fuel and High Flux Isotope Reactor (HFIR) fuel similar to the planned SB11 discard. Following this evaluation, the flowsheet has been slightly altered to address (i) new nuclear criticality safety controls for DWPF that credit a higher amount of gadolinium as a neutron poison for all of the enriched uranium contained in a SB and (ii) potential additions of the H-Canyon neutralized fuel stream prior to the Low Temperature Aluminum Dissolution (LTAD) process in Tank 51. The early introduction of ABD material into the SB assembly process is being investigated to provide flexibility regarding transfer opportunities for H-Canyon to Tank 51 for SB11 and future sludge batches.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Impact of Time Dependent Reactor and Sensor Physics on Core Power Synthesis

Online synthesis of the power distribution is critical in the operation and control of nuclear power reactors to ensure that the core is operating within safety margins, and to provide essential knowledge associated with the burnup of the fuel. In light water reactors (LWRs), power synthesis is achieved by using some a priori knowledge of the state of the reactor core and updating based on the signals coming from in-core sensors—namely, self-powered neutron detectors (SPNDs). This report aims to study the effects of fuel burnup and sensor degradation on the ability to accurately synthesize the power distribution in a LWR. Several modeling tools were used to simulate power synthesis based on the responses of SPNDs, with emitters made out of Rh or V. A representative pressurized water reactor low-enriched uranium (LEU) core was modeled using the Polaris/Purdue Advanced Reactor Core Simulator (PARCS) approach. The Monte Carlo N-Particle Transport 6 (MCNP6) code was used, as well, to calculate response functions between different segments of fuel to individual SPNDs; this is a crucial parameter for power synthesis. The Oak Ridge Isotope GENeration (ORIGEN) package in the Standardized Computer Analyses for Licensing Evaluation (SCALE) code was used to model the time-dependent isotopic transmutation in the SPND emitters. All these data were fed into a custom code that enacted the point-based iterative (PBI) method to simulate power synthesis. Developmental work was also performed on high-fidelity SPND models in the GEometry ANd Tracking 4 (Geant4) code, which enables higher-accuracy modeling of the current responses from SPNDs. In this work, five sets of time-dependent power synthesis test cases were conducted. In these test cases, systematic changes in the input conditions enabled an analysis of the effect of (1) slightly inaccurate a priori power distribution assumptions with respect to fuel burnup, (2) highly inaccurate a priori assumptions with respect to fuel burnup (such that burnup is not included in the a priori assumed distribution), and (3) differences between Rh and V SPNDs in terms of downstream consequences of the transmutation in the emitters. The authors discovered that one may permissibly have slightly inaccurate a priori assumptions of the fuel burnup (such that the level of burnup may be slightly under- or over-approximated by the accumulated burnup in approximately 9.3 full power days), but to not account for burnup at all in the a priori assumption leads to severe levels of error, approaching 25% at maximum. The authors also discovered that V SPNDs are extraordinarily robust in the low-enriched uranium fuel cycle considered in this modeling work, whereas Rh SPNDs undergo significant transmutation that can result in large errors in the synthesized power distribution.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2024

A compact furnace to support in situ neutron imaging of hydrogen dynamics in yttrium hydride moderators

A compact, nuclear microreactor that utilizes low-enriched uranium fuel is a promising solution to meet U.S. energy demands in nonconventional nuclear markets such as remote and decentralized energy grids. Yttrium hydride (YHx) is a potential moderator material for a microreactor design that reduces the amount of required fuel and provides superior retention of hydrogen at high reactor operating temperatures. Hydrogen diffusion properties in YHx are highly sought after for computer model validation and reactor prototyping. To characterize hydrogen diffusion, a compact dual-zone furnace was developed at Los Alamos National Laboratory and analyzed via neutron imaging at the Los Alamos Neutron Science Center (LANSCE). The goal of these measurements is to assess hydrogen diffusion in YHx samples as a function of applied temperature gradients. Included herein is recent progress in technique and furnace developments as well as initial results from concentration- and temperature-gradient measurements at LANSCE.

Torres, James↗
DOE OSTI2021

Analytical characterization of laser induced plasmas towards uranium isotopic analysis in gaseous uranium hexafluoride

To perform direct enrichment assay on gaseous uranium hexafluoride (UF 6 ) with laser induced breakdown spectroscopy (LIBS), the dominant spectral-line features, evolution of the signal and background of the U II 424.437 nm line, and its Stark width and shift, were studied as a function of UF 6 gas pressure and pulse energy of a nanosecond Nd:YAG laser. In this work, vapor pressure of UF 6 was found to be the most important parameter for LIBS analysis of gaseous UF 6 . Spectral congestion with numerous U lines of high excitation potential was observed and signal-to-background ratio (SBR) was low for measurements with 80 Torr UF 6 . Only when both UF 6 vapor pressure and laser pulse energy were low, for example, less than 20 Torr pressure and 30 mJ pulse energy, the resultant LIBS spectra from gaseous UF 6 resembled those obtained from solid U samples. The experimental data also suggest that U and F atoms recombine back to UF 6 after the laser pulse. The U emission was found to decay fast with a persistent background signal, degrading SBR with delay time. Systematic positive biases were found for UF 6 enrichment assays performed with the 235 U– 238 U line pair at 424.412–424.437 nm, which was confirmed to be caused by self-absorption. Even with optimization of experimental parameters and incorporation of a self-absorption term into the spectral-fitting algorithm, to reduce and compensate for self-absorption, self-absorption is still a main factor limiting accurate UF 6 enrichment assay. The use of another spectral window which contains no resonance lines is a prospective solution for the self-absorption issue.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗