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Lithium indium diselenide — An advanced material for neutron detection

Here, this paper describes the synthesis, crystal growth, detector fabrication, radiation hardening studies, MCNP modeling, and characterization of lithium indium diselenide or LiInSe 2 . This newly-developed room temperature thermal neutron detector has semiconducting and scintillating properties and it is suitable for neutron detection application. LiInSe 2 was synthesized starting from elemental Li, In, Se in two steps due to high reactivity of Li. A single crystal of LiInSe 2 was grown using the Vertical Bridgman method. The room temperature band gap was found to be 2.8 eV using optical absorption measurements. Bulk resistivity was measured at ∼5 × 10 11 Ωcm. Photoconductivity measurements of LiInSe 2 wafers identified a peak in the photocurrent around 445 nm. Nuclear radiation detectors were fabricated from single crystal wafer and the responses to alpha particles at various biases were measured. The mobility-lifetime product was estimated. Gamma irradiation studies were performed with calculated absorbed doses ranging from 0.2126 to 21,262 Gy. The characterization of the two wafers for their scintillator performance was conducted after each irradiation. The gamma irradiation produced a reduction of the light yield that translated to a lower channel number for the centroid of alpha detection spectra. It also showed a considerable reduction of the decay time after the first irradiation. These are the first studies on gamma radiation hardening with this material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterizing the Experiment for Calibration with Uranium (Excalibur) neutron source for use in warhead verification

Neutron sources can play a variety of roles in warhead verification. For transmission radiography, a source of directed high energy neutrons is required, while for applications to detect fissile isotopes, sub-MeV neutrons are preferred. The Excalibur (Experiment for Calibration with Uranium) neutron source has been built and used in a variety of verification-related experiments. Excalibur is based on a commercial deuterium-tritium neutron generator specified and measured to be capable of producing 14 MeV neutrons at rates of up to 8.2 × 10 8 neutrons/s. Here, the generator is enclosed in a carbon-steel 32" diameter, 23.62" high carbon-steel cylinder that moderates the mean neutron energy to under 500 keV. This, in turn, is encased in 5%-borated polyethylene such that the entire assembly is a 48" x 48" box that is 30" tall. For radiographic applications, a narrow, tapered channel in the steel and polyethylene allows 14 MeV neutrons to stream directly from the generator to a test object. Its collimating capability is demonstrated by measuring the neutron flux profile. In the moderated mode of operation, the generator is fully enclosed in the steel, but a large section of the polyethylene is removed, providing a flux of sub-MeV neutrons from a wide range of angles. Neutron angular and spectral measurements using both a nested neutron spectrometer and a commercial liquid scintillator coupled with a 3 He detector show the expected softer neutron spectrum in moderated mode in good agreement with MCNP6 calculations. The gamma-ray spectrum from Excalibur is also in good agreement with MCNP modeling. Based on these findings, the future application of Excalibur in its two configurations is discussed.

Fissile material detection↗

Upgrade of the MIT Linear Electrostatic Ion Accelerator (LEIA) for nuclear diagnostics development for Omega, Z and the NIF

The MIT Linear Electrostatic Ion Accelerator (LEIA) generates DD and D{sup 3}He fusion products for the development of nuclear diagnostics for Omega, Z, and the National Ignition Facility (NIF). Significant improvements to the system in recent years are presented. Fusion reaction rates, as high as 10{sup 7} s{sup -1} and 10{sup 6} s{sup -1} for DD and D{sup 3}He, respectively, are now well regulated with a new ion source and electronic gas control system. Charged fusion products are more accurately characterized, which allows for better calibration of existing nuclear diagnostics. In addition, in situ measurements of the on-target beam profile, made with a CCD camera, are used to determine the metrology of the fusion-product source for particle-counting applications. Finally, neutron diagnostics development has been facilitated by detailed Monte Carlo N-Particle Transport (MCNP) modeling of neutrons in the accelerator target chamber, which is used to correct for scattering within the system. These recent improvements have resulted in a versatile platform, which continues to support the existing nuclear diagnostics while simultaneously facilitating the development of new diagnostics in aid of the National Ignition Campaign at the National Ignition Facility.

43 PARTICLE ACCELERATORS↗

TU-H-BRC-06: Temperature Simulation of Tungsten and W25Re Targets to Deliver High Dose Rate 10 MV Photons

Purpose: To study the impact of electron beam size, target thickness, and target temperature on the ability of the flattening filter-free mode (FFF) treatment head to deliver high-dose-rate irradiations. Methods: The dose distribution and transient temperature of the X-ray target under 10 MeV electron beam with pulse length of 5 microseconds, and repetition rate of 1000 Hz was studied. A MCNP model was built to calculate the percentage depth dose (PPD) distribution in a water phantom at a distance of 100 cm. ANSYS software was used to run heat transfer simulations. The PPD and temperature for both tungsten and W25Re targets for different electron beam sizes (FHWM 0.2, 0.5, 1 and 2 mm) and target thickness (0.2 to 2 mm) were studied. Results: Decreasing the target thickness from 1 mm to 0.5 mm, caused a surface dose increase about 10 percent. For both target materials, the peak temperature was about 1.6 times higher for 0.5 mm electron beam compared to the 1 mm beam after reaching their equilibrium. For increasing target thicknesses, the temperature rise caused by the first pulse is similar for all thicknesses, however the temperature difference for subsequent pulses becomes larger until a constant ratio is reached. The target peak temperature after reaching equilibrium can be calculated by adding the steady state temperature and the amplitude of the temperature oscillation. Conclusion: This work indicates the potential to obtain high dose rate irradiation by selecting target material, geometry and electron beam parameters. W25Re may not outperformed tungsten when the target is thick due to its relatively low thermal conductivity. The electron beam size only affects the target temperature but not the PPD. Thin target is preferred to obtain high dose rate and low target temperature, however, the resulting high surface dose is a major concern. NIH funding:R21 EB015957-01; DOD funding:W81XWH-13-1-0165 BL, PM, PB, and RF are founders of TibaRay, Inc. BL is also a borad member. BL and PM have received research grants from Varian Medical System, Inc. and RaySearch Laboratory. RF is an employee of Siemens Healthcare GmbH.

60 APPLIED LIFE SCIENCES↗

Analysis of activated air following high yield shots in the NIF

During the ignition experimental campaign, the National Ignition Facility (NIF) is expected to perform shots with varying fusion yield (up to 20 MJ or 7.1 x 10 18 neutrons per shot) and a maximum annual yield of 1200 MJ. A detailed MCNP model of the Target Bay (TB) and the two switchyards (SY) has been developed to estimate the post-shot radiation environment inside the facility. During D-T shots, a pulse of 14.1 MeV neutrons streaming outside the Target Chamber (TC) will activate the air present inside the TB and the argon gas inside the laser tubes. Smaller levels of activity are also generated in the SY air and in the argon portion of the SY laser beam path. The activated TB air will be mixed with fresh air from the Operations Support Building (OSB) before release through the stack. Flow of activated air from the Target Bay is controlled by the heating, ventilating, and air conditioning (HVAC) system. 16 N (T 1/2 = 7.13 s) dominates the radiation levels during the first minute following the shot. It is expected that 16 N will decay away during the confinement time before releasing the TB air through the stack. The other major contributors are 13 N (T 1/2 = 9.97 min) and 41 Ar (T 1/2 = 1.83 h). In general a low dose rate of < 1 μSv/h is expected near the stack during the first few hours following a 20 MJ shot. Here, the amount of activated Target Bay air released through the stack is very small and does not pose significant hazard to personnel or the environment. In the mean time, due to a very small leakage rate out of the laser tubes, the activated argon gas decays within the tubes and any resulting release to the environment is insignificant.

61 RADIATION PROTECTION AND DOSIMETRY↗

Fuel Cycle Research & Development: Technical Monthly – June 2012

Topics are: (1) MPACT Campaign - (a) Management and Integration • Coordination meetings between NE and NA-22, NA-24, and NA-82 were conducted the week of June 11th. Preparations are being made for the next MPACT working group meeting, scheduled for Aug 28-30 at Idaho Falls. In addition to covering accomplishments and discussing future plans, a site tour of INL facilities (MFC, EBR, ATR, INTEC) is being organized. (2) Accounting and Control Technologies - (a) Microcalorimetry • Now operating 256-pixel array at LANL. We are in the process of tuning detector parameters to improve and optimize performance. Preliminary measurements show approximate number of live pixels is similar to that observed previously at NIST. Continuing to study contribution to systematic error from uncertainties in tabulated gamma-ray energies. (b) Electrochemical Sensor • Testing of sensors fashioned from different precursor materials continued. SEM analysis of all used sensors has been or will be performed. (c) Lead Slowing Down Spectrometer • Ongoing perturbation calculations are providing information on the fundamental systematic error limits of LSDS. In order to achieve separating the contribution of Pu and 235U to the signal, there will need to be tight controls on systematic errors. Continuing to look into a He4 detector. Research into local construction of a He4 detector continued. We have started to apply the algorithm to test the LSDS using experimental data from previous RPI measurements. PNNL also developed a plan to address the lack of statistics in the MCNP modeling of the NGSI 64 assemblies. The ISU graduate student built and tested a fission chamber to gain experience with them. (d) Fast Neutron Imaging to Quantify Nuclear Materials • The imaging detector design was modified for each pixel to have an 8 x 8 pixel array. Quotations and purchasing process for components, including the new PSD scintillator are in progress. (e) Fast Neutron Multiplicity Analysis • The team submitted two papers to the upcoming INMM meeting that are related to the fast neutron multiplicity R&D effort. Progress was made on the project's main goal of designing a concept for a prototype fast-neutron multiplicity counter. We started laying out the outline for the final report. We have been working with our ORNL collaborators to develop a new digitizer system to support our experimental campaign planned for next year. (3) MPACT Analysis Tools - (a) Multi-isotope Process Monitor • Fuel characterization framework development continued during June. A report describing the methodologies is being completed. Kenneth Dayman, from University of Texas, spent a week at PNNL wrapping up his master's research and working on a journal submission covering that work. The target journal is the IEEE transactions on Nuclear Science; submission is planned for the end of July. A proposal to instrument H-Canyon is being prepared in conjunction with SRNL and the NNSA's NGSI program. The impact of gamma-ray spectrum counting statistics on the precision of relative radioisotope component intensities as reconstructed via Principal Component Regression (PCR) continued in June with Monte Carlo simulations of a two-component (i.e., two radioisotope) system. This work generalizes earlier studies in FY12 in which Poisson counting variations of only a single spectrum component were simulated. (b) Modeling and Simulation for Analysis of Safeguards Performance (Electrochemical) • Preliminary insights into safeguards challenges and the initial design for an electrochemical plant have been written up into an INMM paper and will be presented at the INMM Summer Meeting. Work is currently adding a new visualization capability for integrating materials accountancy with physical protection. (c) Material Control including Process Monitoring (Pattern Recognition, Sensors) • Fabrication of quartz chips continued at an external foundry. Awaiting delivery of the heat exchange manifold and chip holder. (d) MPACT System Integration and Technical Support • The initial report on cost-basis metrics for nuclear material security risk and proliferation risk was completed as scheduled. (4) Safeguards and Security by Design - (a) Used fuels storage security analysis, guidance and best practices • RFP was finalized and sent out. Awaiting response from World Institute for Nuclear Security. Coordinated with Scott Demuth on joint report • LANL milestone on best practices. Attended Nuclear Energy Institute National Nuclear Security Conference. Developed plan for soliciting input on prioritized issues for used fuel storage security. Worked on setting up a meeting with the Nuclear Regulatory Commission. Worked on FY2013 work package planning.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutronics Conversion Analyses of the Laue-Langevin Institute (ILL) High Flux Reactor (RHF)

The following report describes the neutronics results obtained with the MCNP model of the RHF U7Mo LEU reference design that has been established in 2010 during the feasibility analysis. This work constitutes a complete and detailed neutronics analysis of that LEU design using models that have been significantly improved since 2010 and the release of the feasibility report. When possible, the credibility of the neutronics model is tested by comparing the HEU model results with experimental data or other codes calculations results. The results obtained with the LEU model are systematically compared to the HEU model. The changes applied to the neutronics model lead to better comparisons with experimental data or improved the calculation efficiency but do not challenge the conclusion of the feasibility analysis. If the U7Mo fuel is commercially available, not cost prohibitive, a back-end solution is established and if it is possible to manufacture the proposed element, neutronics analyses show that the performance of the reactor would not be challenged by the conversion to LEU fuel.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

2015 In-Situ Gamma-Ray Assay of the West Cell Line in the 235-F Plutonium Fuel Form Facility

In November and December 2015, scientists from SRNL took a series of in-situ gamma-ray measurements through the windows in front of Cells 6-9 on the west line of the PuFF facility using a shielded, 120% high-purity germanium detector. The detector efficiency was estimated using a combination of MCNP simulations and empirical measurements. Where possible, the distribution of the Pu-238 in the cells was determined using the Germanium Gamma-ray Imager (GeGI). This distribution was then fed into the MCNP model to quantify the Pu-238 in each cell. Data analysis was performed using three gamma rays emitted by Pu-238 (99.85 keV, 152.7 keV, and 766.4 keV) providing three independent estimates of the mass of Pu-238 holdup in each of the cells.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Boron-lined parallel-plate Collar

This report presents boron-lined parallel plate technology features, experimental benchmarking of initial MCNP model, and parallel-plate UNCL collar optimization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Transient Simulation of the Multi-SERTTA Experiment with MAMMOTH

This work details the MAMMOTH reactor physics simulations of the Static Environment Rodlet Transient Test Apparatus (SERTTA) conducted at Idaho National Laboratory in FY-2017. TREAT static-environment experiment vehicles are being developed to enable transient testing of Pressurized Water Reactor (PWR) type fuel specimens, including fuel concepts with enhanced accident tolerance (Accident Tolerant Fuels, ATF). The MAMMOTH simulations include point reactor kinetics as well as spatial dynamics for a temperature-limited transient. The strongly coupled multi-physics solutions of the neutron flux and temperature fields are second order accurate both in the spatial and temporal domains. MAMMOTH produces pellet stack powers that are within 1.5% of the Monte Carlo reference solutions. Some discrepancies between the MCNP model used in the design of the flux collars and the Serpent/MAMMOTH models lead to higher power and energy deposition values in Multi-SERTTA unit 1. The TREAT core results compare well with the safety case computed with point reactor kinetics in RELAP5-3D. The reactor period is 44 msec, which corresponds to a reactivity insertion of 2.685% delta k/k$. The peak core power in the spatial dynamics simulation is 431 MW, which the point kinetics model over-predicts by 12%. The pulse width at half the maximum power is 0.177 sec. Subtle transient effects are apparent at the beginning insertion in the experimental samples due to the control rod removal. Additional difference due to transient effects are observed in the sample powers and enthalpy. The time dependence of the power coupling factor (PCF) is calculated for the various fuel stacks of the Multi-SERTTA vehicle. Sample temperatures in excess of 3100 K, the melting point UO$_2$, are computed with the adiabatic heat transfer model. The planned shaped-transient might introduce additional effects that cannot be predicted with PRK models. Future modeling will be focused on the shaped-transient by improving the control rod models in MAMMOTH and adding the BISON thermo-elastic models and thermal-fluids heat transfer.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Project Arrangement NP-06 Feasibility study of the applicability for future advanced Pu direct monitoring technology for Pu solutions with FP at reprocessing plants - Gamma-ray Analysis

This report summarizes the efforts to investigate the gamma-ray radiation signatures present in High Active Liquid (HAL) to determine the feasibility of developing advanced plutonium monitoring technology for plutonium to improve safeguards verification measurements and nuclear material accountancy at the Tokai Reprocessing Plant. This includes the development of MCNP models of a waste tank and ion chamber and using experimental results to benchmark the model. With this model the expected dose rate and gamma radiation signatures could be determined for various volumes of liquid waste in the tank.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Neutronic Comparison of New HSA Cobalt Capsule Design to Legacy HSA Cobalt Capsule Design

A comparison of the neutronic properties between the legacy high specific activity (HSA) cobalt capsule design and the new HSA cobalt capsule design was conducted utilizing the full advanced test reactor core MCNP model. The neutron flux and effective neutron absorption cross section for the desired (n,gamma) reaction as well as the undesired reactions (n,2n), (n, alpha), and (n,p) for the cobalt target material for each design was calculated and compared. It was found that the effective neutron absorption cross section for the desired reaction (n,gamma) on the target material that directly produces Co-60 is slightly higher in the new design than the legacy design, and there is little statistical difference between the two target designs for the undesired reactions (n,2n), (n, ), and (n,p). Based on these results, neutronically, there does not appear to be a significant difference between the two capsule designs.

07 ISOTOPE AND RADIATION SOURCES↗

Activation Foil Report for the June 2016 IER-151NCERC Irradiation

A critical experiment was conducted at NCERC on 6 Jun 2016. In this experiment, two sets of activation foils (Cu, Ni, Sc and Ti) were placed within the core. After the irradiation, the foils were withdrawn, packaged and set to the LANL C-NR Countroom and the foils were counted over a period of a few weeks. The results were tabulated and a simple MCNP model was created to simulate a neutron spectrum consistent with the foil results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Random Variation of ACRR Core Report

The research presented in this paper is to be a contribution to a larger research project. The project was designed to test the safety standards of Sandia National Laboratories' ACRR. The MCNP model of the ACRR core is being used to simulate the environment. To test the safety standards, the dimensions and density of the fuel in the core were varied randomly. Each rod had its own dimension and density assigned to it randomly. Ten different cases of the ACRR core were randomly created. The different cases were studied using 640-group neutron fluxes. The fluxes were compared to see how the variations affected the system.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

GEOMWRITER - A Workflow for Automatically Generating MCNP Geometry for Neutron Guide Simulations

This report describes the functionality of the geomwriter.py script, which is a python script for producing complex MCNP CSG geometries from the IGES CAD format. It is specifically written to handle neutron supermirror guides, but can handle more complex objects through utilizing a convex hull algorithm. This work flow reduces the amount of time spent on generating the surface definitions for a complex neutron guide system with hundreds of segments such that changes to the neutron guide system design in McStas can be rapidly incorporated into an MCNP model and integrated with the shielding geometry present in that model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ratio of 1,275 and 186 keV Gamma Ray Count Rates for Age Determination of Material in UF 6 Cylinders

In this work, a method for using ratios of passive gamma ray measurements to determine the time since the filling of UF 6 cylinders was explored. This method uses the 186 keV gamma ray emitted by 235 U and the 1,275 keV gamma ray that results from interactions of alpha particles in fluorine. Studies were made using MCNP models of both 30B cylinders and smaller 5A cylinders. Results indicate that for enrichments at or above that of natural uranium, this approach may provide a method for determining age up to 10 years or identifying whether the age is greater than 10 years, even if the uranium enrichment is unknown. The calculated results show the same behavior as the results of a recent measurement campaign, indicating the possibility of using this method for real-world cylinders.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Energy Deposition Analysis of VERA Progression Problems using MCNP6

The current energy deposition model in the CASL neutronics code MPACT assumes all the fission energy is deposited locally. This approximation limits the accurate represen tation of the heating source distribution in the reactor core, which is essential for the thermal/hydraulic coupling calculations. There has been ongoing work to develop im proved models in MPACT to account for the energy deposition distribution of gamma rays, including direct fission gamma (prompt and delayed) and the gamma rays from neutron capture. Also, the neutron/photon coupling transport calculation has been considered as a potential capability to be added in MPACT to provide high-fidelity heating calculations. In order to provide a reference solution for these gamma heating models, MCNP has been used in this work to develop a set of energy deposition bench mark problems, based on the elective VERA Progression Problems, including single pin cells, 2-D assemblies and 2-D quarter core cases.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Feasibility of an Active Interrogation System to Classify Waste with He-4 Neutron Spectroscopy

This work investigates a 4 He-detector active interrogation system that leverages neutron spectroscopy to classify nuclear waste streams. MCNP models tested the concept through the simulation of a D-D neutron generator, an array of 4 He detectors, and various waste compositions. The fast-neutron Differential Die-Away signature was augmented with a neutron-energy discrimination signature. This signature isolates induced fission neutrons, the energy of which is greater than that of the D-D monoenergetic spectrum. With the incorporation of this spectroscopic technique, the measurement time decreased by 3–9% (depending on the degree of neutron moderation and absorption presented by the sample), demonstrating how neutron spectroscopy can enhance active interrogation methods. The reduced measurement times would have significant financial and logistical benefits for facilities with large footprints of low-level waste production.

4He detectors↗