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Radiation Characterization Summary: NETL Beam Port 1/5 Free-Field Environment at the 128-inch Core Centerline Adjacent (NETL-FF-BP1/5-128-cca)

This document presents the facility-recommended characterization of the neutron, prompt gamma ray, and delayed gamma ray radiation fields in the University of Texas at Austin Nuclear Engineering Teaching Laboratory (NETL) TRIGA reactor for the beam port 1/5 free-field environment at the 128-inch location adjacent to the core centerline. The designation for this environment is NETL-FF-BP1/5-128-cca. The neutron, prompt gamma ray, and delayed gamma ray energy spectra, uncertainties, and covariance matrices are presented as well as radial and axial neutron and gamma ray fluence profiles within the experiment area of the cavity. Recommended constants are given to facilitate the conversion of various dosimetry readings into radiation metrics desired by experimenters. Representative pulse operations are presented with conversion examples.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiation Characterization Summary: Godiva IV Critical Assembly Environments at the In-Core, Top Hat, 1m, and 2m Irradiation Locations

This document presents the facility-recommended characterization of the neutron, prompt gamma ray, and delayed gamma ray radiation fields at the Godiva IV critical assembly at the National Criticality Experiments Research Center (NCERC). The environments assessed include the In-Core location, a location on the Top Hat, 1m away from the assembly, and 2m away from the assembly. The neutron, prompt gamma ray, and delayed gamma ray energy spectra, uncertainties, and covariance matrices are presented as well as radial and axial neutron and gamma ray fluence profiles on the Top Hat surrounding the critical assembly. Recommended constants are given to facilitate the conversion of various dosimetry readings into radiation metrics desired by experimenters. Representative pulse operations are presented with conversion examples.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Verification of the MC2-3 Gamma Library

The new gamma library was generated based on the 94-group gamma structure, including delayed gamma and beta data, using the PreGAMMA and GenGAMMA codes with ENDF/BVII. 0 data. The new gamma library was first verified using the 2D benchmark problems that were introduced in the GAMSOR manual, showing that the neutron and gamma heatings from DIF3D were in good agreement with MCNP solutions within 5% even in the non-fuel regions of both cores with uranium or plutonium dominant fuel compositions. Similarly, the DIF3D power solutions for additional simpler 1D problems with 3 or 6 regions showed good agreement with MCNP solutions. Note that all DIF3D calculations were based on the 230- group neutron and 94-group gamma data. For the EBR-II benchmark problem, the DIF3D solution with the new gamma library maintained good agreement in the power distribution with the MCNP solution, which is comparable to the DIF3D results with the current 21-group gamma library. The use of delayed gamma and beta data increased powers at the dummy assemblies by 26%, which appears to be reasonable. Further detailed verification tests may be necessary and, more importantly, validation tests are required against measurement data.

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Delayed Gamma-ray Assay for Nuclear Materials Safeguards. Comprehensive Technology Readiness Assessment

Spectroscopic analysis of beta-delayed gamma-rays emitted from fission products following active interrogation was investigated as a non-destructive assay technique for detection and characterization of nuclear materials in shielded and complex configurations. This measurement technique is expected to be applicable to a variety of applications within the nuclear material safeguards, arms control, and emergency response areas, where active neutron interrogation is acceptable. Potential applications of the delayed gamma-ray assay in the nuclear material safeguards area include characterization of U and Pu isotopic content in spent and unirradiated nuclear fuel, enrichment measurements, verification of bulk material in containers, and the characterization of nuclear wastes. In the arms control area, this method can be used as a part of warhead dismantlement measurements to confirm separation of components, and may be applicable in warhead confirmation. In the context of emergency response, it can be used for detailed diagnostics of an unknown item. At present, the delayed gamma-ray assay technology reliably qualifies for the Technical Readiness Level 3 (TRL 3). The R&D work completed under this project has successfully demonstrated the empirical proof-of-concept for this active interrogation technology for a variety of measurement configurations, neutron sources, and nuclear material samples. A robust first-principles analytical signature modeling methodology was developed, experimentally validated, and can be easily extrapolated to a range of realistic measurement scenarios. Several response analysis methodologies have been implemented and deemed reliable for a variety of active interrogation applications in the areas of nuclear material safeguards, arms control, and emergency response. The initial readiness level before the start of this project was assessed at TRL 0, since only fragmentary records of the signature observations and speculative statements of the relevant non-destructive assay applications existed at that time. The delayed gamma-ray technology readiness can be easily advanced to TRL 4 in a short period, if a certain measurement application is specified and set for a demonstration in a laboratory environment. The critical hardware components of the delayed gamma-ray measurement technology (neutron generators, gamma-ray spectrometers) are readily available as COTS and can be configured for a specific deployment configuration. The primary risk of the delayed gamma-ray assay methodology is defined by the applicationspecific uncertainties. Evaluation of the system performance can be effectively completed once the expected measurement purpose, nuclear material characteristics, dimensions, and radiation exposure constraints are specified. A minor risk can be associated with the delayed gamma-ray response analysis techniques. Several approaches were proposed and demonstrated primarily using the modeled signatures. The observed performance may not be easily transferrable to the conditions of a real measurement setup, and some additional R&D may be required. Overall, the delayed gamma-ray assay technology can be recommended for follow-up demonstrations addressing relevant measurement applications in the areas of nuclear material safeguards, arms control, and emergency response.

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Beta Decay Study of the T{sub z}=−2{sup 56}Zn Nucleus and the Determination of the Half-Lives of a Few fp-shell Nuclei

This paper concerns the experimental study of the β decay properties of few proton-rich fp-shell nuclei. The nuclei were produced at GANIL in fragmentation reactions, separated with the LISE spectrometer and stopped in an implantation detector surrounded by Ge detectors. The β-delayed gammas, β-delayed protons and the exotic β-delayed gamma-proton emission have been studied. Preliminary results are presented. The decay of the T{sub z}=−2 nucleus {sup 56}Zn has been studied in detail. Information from the β-delayed protons and β-delayed gammas has been used to deduce the decay scheme. The exotic beta-delayed gamma-proton decay has been observed for the first time in the fp-shell. The interpretation of the data was made possible thanks to the detailed knowledge of the mirror Charge Exchange (CE) process and the gamma de-excitation of the states in {sup 56}Co, the mirror nucleus of {sup 56}Cu.

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DN/DG Screening of Environmental Swipe Samples: FY2016 Report

The Delayed Neutron Delayed Gamma (DNDG) technique provides a new analytical capability to the International Atomic Energy Agency (IAEA) for detecting undeclared nuclear activities. IAEA’s Long Term R&D (LTRD) plan has a stated high urgency need to develop elemental and isotopic signatures of nuclear fuel cycle activities and processes (LTRD 2.2). The new DNDG capability is used to co-detect both uranium and plutonium as an extension of a DN only method that is already being utilized by the IAEA for the analysis of swipes to inform on undeclared nuclear activities. Analytical method involving irradiation of swipe samples potentially containing trace quantities of fissile material in a thermal neutron field, followed by the counting of delayed neutrons, is a well-known technique in the field of safeguards and nonproliferation. It is used for detecting the presence of microscopic amounts of fissile material, (typically a linear combination of 233 U, 235 U, 239 Pu, and 241 Pu)and quantifying it in terms of the equivalent mass of 235U. The delayed neutron (DN) technique is very sensitive and is been routinely employed at the High Flux Isotope Reactor (HFIR) facility at Oak Ridge National Laboratory (ORNL). Both uranium and plutonium are of high safeguards value. However, the DN technique is not well suited for distinguishing between U and Pu isotopes since the decay curves overlap closely. The delayed gamma (DG) technique will help detect the presence of 239Pu in a mixture of U and Pu. Thus the DNDG approach combines the best of both worlds; the sensitivity of DN counting and the isotopic specificity of DG counting. The present work seeks to build on the delayed neutron and delayed gamma methods that have been developed at ORNL. It is recognized that the distribution profile of heavy fission products remains fairly invariant for the fissile nuclides whereas the distribution of light fission products varies from one isotope to another. That is, the ratio of the yield of a light fission fragment to a heavy fission fragments is isotope specific. Measurement of the ratio of the net full energy peak (FEP) from low/high mass fission products is an elegant way to characterize the fraction of fissile materials present in a mixture. By empirically calibrating the ratio of the net FEP as a function of known concentration of the binary mixture, one can determine the fraction of fissile isotopes in an unknown sample. In the work done in fiscal year (FY) 2016, samples of single fissile material isotopes as well as binary mixtures were irradiated in a well thermalized irradiation field in the HFIR. Delayed neutron counting was performed using the neutron counter at the HFIR Neutron Activation Analysis (NAA) laboratory. Delayed gamma counting was performed using a shielded high purity germanium (HPGe) detector. Delayed neutron decay curve results highlighted the difficulty of distinguishing between U and Pu isotopes, and the need for including the delayed gamma component. Based on delayed gamma spectrometry, twelve ratios of low mass/high fission product gamma ray FEP have been identified as valid candidates. Linearity of the ratios, as a function of 239 Pu fraction in 235 U+ 239 Pu mixtures, was confirmed for the low mass/high mass candidates that were selected. The DNDG method we are spearheading allows not only the presence of total fissile content to be detected, but whether the material is predominantly U or predominantly Pu, or a mixture. This provides additional SG relevant information.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

This project has been a collaborative effort of researchers from four National Laboratories, Lawrence Berkley National Laboratory (LBNL), Lawrence Livermore National Laboratory (LLNL), Los Alamos National Laboratory (LANL), Pacific Northwest National Laboratory (PNNL), and Idaho State University’s (ISU) Idaho Accelerator Center (IAC). Experimental measurements at the Oregon State University (OSU) were also supported. The research included two key components, a strong experimental campaign to characterize the delayed gamma-ray signatures of the isotopes of interests and of combined targets, and a closely linked modeling effort to assess system designs and applications. Experimental measurements were performed to evaluate fission fragment yields, to test methods for determining isotopic fractions, and to benchmark the modeling code package. Detailed signature knowledge is essential for analyzing the capabilities of the delayed gamma technique, optimizing measurement parameters, and specifying neutron source and gamma-ray detection system requirements. The research was divided into three tasks: experimental measurements, characterization of fission yields, and development of analysis methods (task 1), modeling in support of experiment design and analysis and for the assessment of applications (task 2), and high-rate gamma-ray detector studies (task 3).

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Delayed Gamma-ray Assay for Nuclear Materials Safeguards: Additional Tasks

This report documents the activities and findings completed under the extended task scope in FY17-18. This work was performed as a follow-up to the original effort that investigated the delayed gamma-ray signatures of nuclear materials and was a collaborative effort between Lawrence Livermore, Lawrence Berkeley, Los Alamos National Laboratories and the Idaho Accelerator Center. The original project was focused on the delayed gamma-ray (DG) assay application for spent nuclear fuel safeguards, as a methodology to directly quantify the content and composition of U and Pu isotopes in irradiated assemblies in storage or before transfer to a difficult-to-access repository.

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Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

Modeling capabilities were added to an existing framework and codes were adapted as needed for analyzing experiments and assessing application-specific assay concepts including simulation of measurements over many short irradiation/spectroscopy cycles. The code package was benchmarked against the data collected at the IAC for small targets and assembly-scale data collected at LANL. A study of delayed gamma-ray spectroscopy for nuclear safeguards was performed for a variety of assemblies in the extensive NGSI spent fuel library. The modeling results indicate that delayed gamma-ray responses can be collected from spent fuel assemblies with statistical quality sufficient for analyzing their isotopic composition using a 10 11 n/s neutron generator and COTS detector instrumentation.

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FIER: Software for analytical modeling of delayed gamma-ray spectra

We report a new software package, the Fission Induced Electromagnetic Response (FIER) code, has been developed to analytically predict delayed γ-ray spectra following fission. FIER uses evaluated nuclear data and solutions to the Bateman equations to calculate the time-dependent populations of fission products and their decay daughters resulting from irradiation of a fissionable isotope. These populations are then used in the calculation of γ-ray emission rates to obtain the corresponding delayed γ-ray spectra. FIER output was compared to experimental data obtained by irradiation of a 235 U sample in the Godiva critical assembly. This investigation illuminated discrepancies in the input nuclear data libraries, showcasing the usefulness of FIER as a tool to address nuclear data deficiencies through comparison with experimental data. Finally, FIER provides traceability between γ-ray emissions and their contributing nuclear species, decay chains, and parent fission fragments, yielding a new capability for the nuclear science community.

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Method for Calculating Delayed Gamma-Ray Response in the ACRR Central Cavity and FREC-II Cavity Using MCNP

This document presents the process for a new method developed for the characterization of the delayed gamma-ray radiation fields in pulse reactors like the Annular Core Research Reactor (ACRR) and the Fueled Ring External Cavity (FREC-II). The environments used to test this method in the ACRR were FF, LB44, PLG and CdPoly, and the environments used in the FREC-II were FF with rods-down, FF with rods-up, CdPoly with rods-down and CdPoly with rods-up. All environment configurations used the same fission product gamma-ray source energy spectrum. This method required the fission sites located in the MCNP KCODE source tapes. A FORTRAN script was written to translate and extract the coordinates for the fission sites. The 10K fission sites were then input it into an MCNP SOURCE mode script. Using a MATLAB script, a parametric analysis was done, and it helped determine that 10K fission sites are an appropriate number of coordinates to converge to the correct answer. The method gave excellent results and was tested in the ACRR, FREC-II and White Sands Missile Range (WSMR). This method can be applied to other pulse research reactors as well.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Delayed Gamma-ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

This project addresses the need for improved non-destructive assay techniques for quantifying the actinide composition of spent nuclear fuel and for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle. High-energy delayed gamma-ray spectroscopy following neutron irradiation is a potential technique for directly assaying spent fuel assemblies and achieving the safeguards goal of quantifying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Delayed gamma-ray spectroscopy with lanthanum bromide detector for non-destructive assay of nuclear material

High-energy delayed γ-ray spectroscopy is a potential technique for directly assaying spent fuel assemblies and achieving the safeguards goal of quantifying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Requirements for the γ-ray detection system, up to ~6 MeV, can be summarized as follows: high efficiency at high γ-ray energies, high energy resolution, good linearity between γ-ray energy and output signal amplitude, ability to operate at very high count rates, and ease of use in industrial environments such as nuclear facilities. High Purity Germanium Detectors (HPGe) are the state of the art and provide excellent energy resolution but are limited in their count rate capability. Lanthanum Bromide (LaBr 3 ) scintillation detectors offer significantly higher count rate capabilities at lower energy resolution. Thus, LaBr 3 detectors may be an effective alternative for nuclear spent-fuel applications, where count-rate capability is a requirement. This paper documents the measured performance of a 2” (length) × 2” (diameter) of LaBr3 scintillation detector system, coupled to a negatively biased PMT and a tapered active high voltage divider, with count-rates up to ~3 Mcps. An experimental methodology was developed that uses the average current from the PMT’s anode and a dual source method to characterize the detector system at specific very high count rate values. Delayed γ-ray spectra were acquired with the LaBr 3 detector system at the Idaho Accelerator Center, Idaho State University, where samples of ~3g of 235 U were irradiated with moderated neutrons from a photo-neutron source. Results of the spectroscopy characterization and analysis of the delayed γ-ray spectra acquired indicate the possible use of LaBr3 scintillation detectors when high count rate capability may outweigh the lower energy resolution.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

User Manual for MC2-3 Gamma Library Generation

This document presents a detailed description of generating the gamma library for MC 2 -3 which includes delayed gammas and betas based on the 94 gamma energy groups. The updated methodologies associated with heating and gamma calculations are introduced, which account for the self-shielding effect on KERMA factors and perform the gamma transport calculations to condense the gamma data from 94 to 21 groups. For these updates, the PreGAMMA code was developed to prepare NJOY inputs and generate delayed gammas and betas, and the GenGAMMA code was updated to process the outputs of PreGAMMA and NJOY. This document briefly discusses verification results of the new gamma library using the ABTR fuel pin and the EBR-II benchmark problem.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improved Gamma Yield and Interaction Cross-Section Libraries of MC2-3

The MC{sup 2}-3 code developed by Argonne National Laboratory (ANL) has been widely used for multigroup cross section generation for fast reactor design and analysis. The neutron cross sections generated with MC{sup 2}-3 have been validated with various fast critical experiments. The gamma production data and interaction cross sections were also verified with the EBR-II benchmark problem. The current gamma calculation process is based on the 21-group gamma libraries generated with the NJOY code, which does not include the delayed gamma production and does not account for the self-shielding effect on the KERMA (Kinetic Energy Released in Material) factor. In order to improve gamma prediction accuracy, the gamma libraries of MC{sup 2}-3 have recently been extended from 21 to 94 groups, including delayed gamma data and kinetic energy release per reaction data. The latter is used to take into account the self-shielding effect on KERMA factors. Gamma transport calculation capabilities have also been added to MC{sup 2}-3. In this paper, we present the updated data and gamma transport capabilities along with the verification tests with ABTR and EBR-II benchmark problems. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

A system for the measurement of delayed neutrons and gammas from special nuclear materials

The delayed neutron counting (DNC) system at the Royal Military College of Canada has been upgraded to accommodate concurrent delayed neutron and gamma measurements. This delayed neutron and gamma counting (DNGC) system uses a SLOWPOKE-2 reactor to irradiate fissile materials before their transfer to a counting arrangement consisting of six ³He and one HPGe detector. The application of this system is demonstrated in an example where delayed neutron and gamma emissions are used in complement to examine ²³³U content and determine fissile mass with an average relative error and accuracy of -2.2 and 1.5 %, respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Applied radiation tags for warhead dismantlement transparency

Here, this study explores the feasibility of applying radiation tags as a Chain of Custody tool to confirm the dismantlement of individual warheads by investigating time dependent emissions from special nuclear material. Precedents of photon and neutron sources that have been used to irradiate warhead components are presented. Measurements of irradiated Highly Enriched Uranium (HEU) are used to benchmark simulations with the CINDER90 library for MCNP. Delayed gamma emissions are simulated as a function of time since irradiation of moderated HEU and Weapons Grade Plutonium with photon and neutron sources. Models of commercial 9 MV and 15 MV linacs were found to induce ~10 9 fissions/g and ~10 11 fissions/g, respectively, creating 3 to 4 orders of magnitude more delayed gammas than neutron sources, modeled at 10 10 n/s. However, a DT neutron source was found to induce sufficient fissions, ~10 7 fissions/g, to create quantifiable signatures relative to intrinsic emissions. Applied radiation tagging is determined to be technically feasible, but its operational context and practical implementation requires significant development.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Annular Core Research Reactor (ACRR) Pulse Curve Characterization

Reactor pulse characterization at the Annular Core Research Reactor (ACRR) at Sandia Technical Area V (TA-V) is commonly done through photo conductive detection (PCD) and calorimeter detectors. Each of these offer a mode of analyzing a digital signal with different advantages/methods for determination of integrated dose or temporal based metrology. This report outlines a method and code that takes the millions of data points from such detectors and delivers a characteristic pulse trendline through two main methods: digital signal filtration and machine learning, in particular, Support Vector Machines (SVMs). Each method's endpoint is to deliver a characteristic curve for the many bucket environments of ACRR while considering other points of interest including delayed gamma removal for prompt dose metrics. This work draws and adds on previous work detailing the delayed gamma fraction contributions from CINDER simulations of the ACRR. Results from this project show a method to determine characteristic curves in a way that has previously been limited by data set size.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗