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At least 19 records

Development of a High-Energy Neutron Sniffer and Subsequent Dose Quantification for High-Energy Particle Accelerator Shielding Surveys

The objective of this research is to design a portable neutron detector that is lightweight and responds to neutrons with energies of 20 MeV and greater. The instrument will be used as a ‘sniffer’ probe for identifying shielding weaknesses at high-energy particle accelerators and be paired with a plastic scintillator to quantify the high-energy neutron dose equivalent. The sniffer probes are two different sizes and comprised of either cesium iodide or sodium iodide, all doped with thallium, making a total of four detectors. The probes were calibrated to respond only to radiations with 8 MeV electron equivalent energy or higher, vastly reducing detector response from background and lower energy radiations. The sniffer probes were tested using californium- 252 and americium-beryllium sources, followed by high-energy (up to 800 MeV) neutron exposures at the Los Alamos Neutron Science Center Weapons Neutron Research (WNR) facility. The sniffer probes were then used to identify areas around the accelerator facility where elevated levels of high-energy radiation was present and the plastic scintillators were placed in these locations to determine the high-energy neutron dose equivalent. The dose equivalent is calculated by measuring the 12 C(n,2n) 11 C reaction, which has a 20.4 MeV neutron threshold. Two locations behind the WNR facility were identified with the probes and the dose equivalent rates from neutron energies above 20 MeV were calculated to be 1.24 mrem/h behind flightpath 30-left and 1.53 behind flightpath 30-right. Of the four sniffer probes, the 2-inch x 2-inch cesium iodide is the recommended probe for performing high-energy shielding surveys. The larger crystal size yields higher sensitivity at lower count rates and the more dense material increases the likelihood of interaction within the crystal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Retrieval, Disposal, and Disposition of Legacy 252 Cf Sealed Sources

In this article, we describe work performed on behalf of the US Department of Energy (DOE) to disposition 467 government-owned, sealed californium-252 ( 252 Cf) sources located at 52 academic and government research sites. These sources are the legacy of the DOE 252 Cf Loan/Lease Program, which operated from the late 1960s until 2008, when the loan program closed abruptly. Although the DOE took decades to fabricate and distribute the sources, best safety and nuclear accountability practices demanded retrieval or disposition of all loaned sources as soon as achievable after the loan program was closed. An adaptable disposition approach was developed, and disposition of the sources was pursued. The approach involved a combination of source retrievals, disposal actions, and source ownership transfers. A new shielded shipping container was designed and deployed to aid in source retrievals. In a couple cases, incomplete source fabrication and shipping records prevented shipment, and those sources were left indefinitely with the customer in a safe configuration. Lastly, all the sources in the inventory were safely dispositioned in some way, and lessons learned from this effort are provided.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Coaxial Fission of Nuclei to Three Commensurate Fragments

Trajectory calculations of the angular distribution of fragments originating from the spontaneous true ternary fission of {sup 252}Cf nuclei are performed with allowance for the rotation of the fissile-nucleus axis. This rotation arises upon scission because of the formation of fragment spins despite the conservation of zero total angular momentum at all fission stages. The calculations in question lead to the conclusion that a collinear tripartition is the most probable in spontaneous true ternary fission of {sup 252}Cf nuclei. This confirms experimental data, thereby creating the basis that is necessary for obtaining deeper insight into them.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Recent applications of nuclear track emulsion technique

A survey of recent results obtained using the nuclear track emulsion (NTE) technique in low energy applications is given. NTE irradiation with 60 MeV {sup 8}He nuclei provides identification of their decays at stopping, evaluation of the possibility of α range spectrometry, and observation of drift of thermalized {sup 8}He atoms. Correlations of α particles studied in {sup 12}C → 3α splitting induced by 14.1 MeV neutrons indicate the presence of a superposition of 0{sup +} and 2{sup +} states of the {sup 8}Be nucleus in the ground state of {sup 12}C. Angular correlations of fragments are studied in boron-enriched NTE, and the prospects of NTE application in radioactivity and nuclear fission research are discussed. It is proposed to use an automated microscope to search for collinear tripartition of heavy nuclei implanted in NTE. Surface irradiation of NTE by a {sup 252}Cf source is started. Planar events containing fragment pairs and long range α particles, as well as fragment triples, are studied. NTE samples are calibrated using Kr and Xe ions with an energy of 1.2 and 3 A MeV.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Sensitivity Coefficients for Diffusion Coefficients and Other Reactor Physics Parameters using CE TSUNAMI-3D

The TSUNAMI (Tools for Sensitivity and Uncertainty Analysis Methodology Implementation) capabilities within the SCALE code system leverage sensitivity coefficients for many criticality safety applications, including quantifying the data-induced uncertainty in the eigenvalue of critical systems, quantifying computational biases, and selecting applicable benchmark experiments. TSUNAMI sensitivity and uncertainty analysis tools have traditionally been limited to criticality safety application spaces, but the introduction of Generalized Perturbation Theory (GPT) sensitivity methods by Jessee in 2009 and Perfetti in 2013 has extended the scope of SCALE adjoint-weighted sensitivity and uncertainty analysis to include reactor physics applications. The continuous-energy (CE) TSUNAMI-3D GPT sensitivity analysis methods were originally developed to calculate sensitivity coefficients for a limited number of reaction-rate responses using CE Monte Carlo methods. These tools were recently applied in an Oak Ridge National Laboratory (ORNL)-directed research and development project to improve the efficiency of {sup 252}Cf production in the High Flux Isotope Reactor (HFIR) by understanding the sensitivity of key heavy actinide capture-to- fission ratios to potential system design changes. This work further extends the applicability of the CE TSUNAMI- 3D GPT methods to reactor physics applications by enabling the calculation of sensitivity coefficients for an expanded set of reaction rate responses-including a first-ever capability for conducting sensitivity analysis of neutron diffusion coefficients.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Experimental determination of the yield of “scission” neutrons from the spontaneous fission of {sup 252}Cf

Angular and energy distributions of prompt neutrons from the spontaneous fission of {sup 252}Cf have been measured. The yield of “scission” neutrons has been estimated by comparing the measured distributions with calculations within the model of emission of neutrons from completely accelerated fragments. It has been shown that the best description of measured angular and energy distributions of fission neutrons is achieved under the assumption that neutrons with a higher (about 6–8%) probability are emitted along the fission axis in the center-of-mass system of fission fragments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Key metrics for HFIR HEU and LEU models

This report compares key metrics for two fuel design models of the High Flux Isotope Reactor (HFIR). The first model represents the highly enriched uranium (HEU) fuel currently in use at HFIR, and the second model considers a low-enriched uranium (LEU) interim design fuel. Except for the fuel region, the two models are consistent, and both include an experiment loading that is representative of HFIR's current operation. The considered key metrics are the neutron flux at the cold source moderator vessel, the mass of 252 Cf produced in the flux trap target region as function of cycle time, the fast neutron flux at locations of interest for material irradiation experiments, and the reactor cycle length. These key metrics are a small subset of the overall HFIR performance and safety metrics. They were defined as a means of capturing data essential for HFIR's primary missions, for use in optimization studies assessing the impact of HFIR's conversion from HEU fuel to different types of LEU fuel designs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Modeling and Depletion Simulations for a High Flux Isotope Reactor Cycle with a Representative Experiment Loading

The purpose of this report is to document a high-fidelity VESTA/MCNP High Flux Isotope Reactor (HFIR) core model that features a new, representative experiment loading. This model, which represents the current, high-enriched uranium fuel core, will serve as a reference for low-enriched uranium conversion studies, safety-basis calculations, and other research activities. A new experiment loading model was developed to better represent current, typical experiment loadings, in comparison to the experiment loading included in the model for Cycle 400 (operated in 2004). The new experiment loading model for the flux trap target region includes full length 252 Cf production targets, 75 Se production capsules, 63 Ni production capsules, a 188 W production capsule, and various materials irradiation targets. Fully loaded 238 Pu production targets are modeled in eleven vertical experiment facilities located in the beryllium reflector. Other changes compared to the Cycle 400 model are the high-fidelity modeling of the fuel element side plates and the material composition of the control elements. Results obtained from the depletion simulations with the new model are presented, with a focus on time-dependent isotopic composition of irradiated fuel and single cycle isotope production metrics.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Status of neutron diagnostics on the experimental advanced superconducting tokamak

Neutron diagnostics have become a significant means to study energetic particles in high power auxiliary heating plasmas on the Experimental Advanced Superconducting Tokamak (EAST). Several kinds of neutron diagnostic systems have been implemented for time-resolved measurements of D-D neutron flux, fluctuation, emission profile, and spectrum. All detectors have been calibrated in laboratory, and in situ calibration using {sup 252}Cf neutron source in EAST is in preparation. A new technology of digitized pulse signal processing is adopted in a wide dynamic range neutron flux monitor, compact recoil proton spectrometer, and time of flight spectrometer. Improvements will be made continuously to the system to achieve better adaptation to the EAST’s harsh γ-ray and electro-magnetic radiation environment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Investigation of Ternary Fission of {sub 98}{sup 252}Cf Using Three-Cluster and Unified Ternary Fission Models

Using three-cluster and unified ternary fission models, the ternary fission of {sub 98}{sup 252}Cf is studied. We applied collinear and equatorial configurations to study the ternary fission of {sub 98}{sup 252}Cf when the third fragment is {sub 3}{sup 10}Li. The nuclear potential energy in the three-cluster model and unified ternary fission model is calculated respectively, using Yukawa plus exponential and proximity formalisms. The relative yields of different fragmentation channels are calculated. Our results reveal that the ternary fragmentation potential of the three fragments and the relative yields depend on the configuration of three fragments and usedmodel. Two models predict that the lowest driving potential and highest relative yield take place for the fragment combination {sub 51}{sup 132}Sb + {sub 44}{sup 110}Ru + {sub 3}{sup 10}Li. Also, the values of driving potential and relative yield are not equal in the three-clustermodel and unified ternary fission model. For fragment combination {sub 51}{sup 132}Sb + {sub 44}{sup 110}Ru + {sub 3}{sup 10}Li, the relative yield based on the three-cluster model in collinear configuration is maximum, whereas the unified ternary fission model in equatorial configuration predicts the lowest relative yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

FREYA Developments 2015-2016

We have been studying the sensitivity of neutron observables to the FREYA input distributions. Patrick Talou generated 1000 different yield functions, Y(A,Z,TKE), for 252 Cf(sf) based on fits to available data on the yields as a function of fragment mass, Y(A), and the total kinetic energy distribution as a function of heavy fragment mass, TKE(AH), and its width, σTKE(AH), to obtain Y(A,TKE). These results are augmented by Wahl systematics to include the fragment charge. We have so far found that the neutron observables do not depend strongly on the yield functions. We also found that the yield functions, constrained by data, are not sufficient to constrain the average neutron multiplicity within the evaluated uncertainty. A paper on this is in progress. We began working on a paper on photofission with the University of Michigan while on a Consortium for Verification Technology fellowship. This is an important paper because they have measured the neutron multiplicity distribution, the prompt fission neutron spectrum, and the energy correlation of two neutrons as a function of angle of separation for the first time in photofission of 235 U. We have made FREYA calculations to compare with the data, but the paper is still in progress since the student left and other researchers have had to take over the analysis. We expect to submit the paper in the next several months, after the analysis is complete.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Verification of Special Nuclear Material (SNM) using Active Well Coincidence Counter (AWCC) and a High Purity Germanium (HPGe) Detector

SNM verification can be accomplished via two methods i.e. destructive analysis (DA) or nondestructive analysis (NDA). The DA modes are much more accurate compared to NDA modes; nevertheless, the sample's physical integrity is destroyed in the process. Techniques such as ICP-MS, ID-ICP-MS, TI-MS are few examples of DA, where a bulk material is ground and mixed with a solution (some form of acid) to acquire a homogenous sample. In contrast, NDA modes utilize signals emitted by the sample such as gamma, neutrons, light, or heat to analyze samples under investigation. HPGe detectors are some of the most frequently used gamma detectors to assay SNM. However, in a high activity scenario it provides a large uncertainty and sometimes becomes unfeasible to measure low energy gamma rays. Meanwhile, neutron detectors are not affected by the gamma background, therefore they can be used in addition to the gamma detectors to verify total fissile mass ({sup 235}U + {sup 239}Pu) of SNM. The AWCC is one of the thermal neutron NDA systems developed at the Los Alamos National Laboratory (LANL). It consists of 42 {sup 3}He detectors to measure gross neutrons (singles), coincidence neutrons (doubles), higher order multiplicity counting (triples, quadruples, etc.). It can effectively operate in both active and passive neutron interrogation modes. It can utilize AmLi, AmBe, or {sup 252}Cf active interrogation neutron sources. It is used to verify declared fissile mass ({sup 235}U or {sup 239}Pu) present in SNM. Objectives: Calibrate HPGe and AWCC for lightly irradiated (with enough {sup 137}Cs gamma background) ∼93% enriched HEU fuels; Verify fissile mass ({sup 235}U +{sup 239}Pu) content using AWCC and HPGe; Model and benchmark AWCC in MCNP6. Neutron coincidence and multiplicity counting: Two or more neutrons are coincident if they are detected by the system within the specified gate window; In AWCC: Gate window is 128 μsec; Induced fission in fissile material such as {sup 235}U and {sup 239}Pu - emission of time correlated neutrons - Singles, Doubles, Triples, or Quadruples; No induced fission in non-fissile materials- no correlated neutrons - only singles. SNM can be verified with high accuracy and precision using gamma and neutron NDA instruments such as HPGe and AWCC. Interaction with thermal neutrons. Non-fissile atoms - do not emit correlated neutrons. Fissile atoms - emit correlated neutrons during induced fission events. The time correlated neutrons can be detected by using coincidence or multiplicity counters such as AWCC. Likewise, {sup 235}U produces 186 keV gamma peak that can be measured by a HPGe gamma detector. Counts under 186 keV gamma peak provide information about {sup 235}U content. Combining AWCC and HPGe results can provide better understanding of special nuclear material under investigation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Realization of highly efficient hexagonal boron nitride neutron detectors

Here, we report the achievement of highly efficient 10 B enriched hexagonal boron nitride (h- 10 BN) direct conversion neutron detectors. These detectors were realized from freestanding 4-in. diameter h- 10 BN wafers 43 μm in thickness obtained from epitaxy growth and subsequent mechanical separation from sapphire substrates. Both sides of the film were subjected to ohmic contact deposition to form a simple vertical “photoconductor-type” detector. Transport measurements revealed excellent vertical transport properties including high electrical resistivity (>10 13 Ω cm) and mobility-lifetime (μτ) products. A much larger μτ product for holes compared to that of electrons along the c-axis of h- BN was observed, implying that holes (electrons) behave like majority (minority) carriers in undoped h- BN. Exposure to thermal neutrons from a californium-252 ( 252 Cf) source moderated by a high density polyethylene moderator reveals that 43 μm h- 10 BN detectors possess 51.4% detection efficiency at a bias voltage of 400 V, which is the highest reported efficiency for any semiconductor-based neutron detector. The results point to the possibility of obtaining highly efficient, compact solid-state neutron detectors with high gamma rejection and low manufacturing and maintenance costs.

36 MATERIALS SCIENCE↗

Isotope Program Report June FY2016

Isotope Program Monthly Highlights are briefly described. These include data on isotopes shipped, updates on equipment fabrication and testing, a potential new approach for nondestructive measurement of the amount of Cf-252 deposited on a surface, and efforts to recover and purify uranium-234 obtained from old PuBe sources.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Benchmarking Data for the Proposed Signature of Used Fuel Casks

A set of benchmarking measurements to test facets of the proposed extended storage signature was conducted on May 17, 2016. The measurements were designed to test the overall concept of how the proposed signature can be used to identify a used fuel cask based only on the distribution of neutron sources within the cask. To simulate the distribution, 4 Cf-252 sources were chosen and arranged on a 3x3 grid in 3 different patterns and raw neutron totals counts were taken at 6 locations around the grid. This is a very simplified test of the typical geometry studied previously in simulation with simulated used nuclear fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Separation and Purification of Berkelium-249 and Einsteinium-254

Berkelium-249 ( 249 Bk) and einsteinium-254 ( 254 Es) are isotopes of great importance for the investigation of berkelium and einsteinium chemical properties and super heavy element research. Therefore, it is necessary to be able to isolate acceptable, pure quantities of both isotopes to further research capabilities. These isotopes, along with californium-252 ( 252 Cf), are synthesized through the irradiation of mixed-curium targets in the High Flux Isotope Reactor (HFIR), which has the highest continuous thermal neutron flux in the world. Once irradiated, the targets are transferred to the Radiochemical Engineering Development Center for further chemical processing and final purification to separate 249 Bk and 254 Es from the remainder of isotopes present. Several methods of separation, such as the Berkex batch solvent extraction along with cation-exchange and alpha-hydroxy-isobutyrate (AHIB) columns, are employed to achieve a clean separation of the isotopes. Production Campaigns 74–77 are discussed in depth for 252 Cf, 249 Bk, and 254 Es production and isolation of 249 Bk and 254 Es. An attempt to isolate 257 Fm in Campaign 77 is discussed as well. Table 1 summarizes the total amount of material isolated in each campaign.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Hot Cell Manipulator Inventory and Recommendations

During the spring of 2021 repeated manipulator failures in the hot cells of Building 7920 contributed to significant delays in Californium-252 ( 252 Cf) mission execution and loss of rapidly decaying 252Cf product. At the same time, funds became available in the 252 Cf program budget for equipment purchases and upgrades. Accordingly, the 252 Cf program manager requested (1) an inventory of the manipulators used in six Oak Ridge National Laboratory (ORNL) buildings (7920, 7930, 4501, 3047, 3025E, and 3525), (2) an inventory of spare manipulators, and (3) a recommendation on whether to invest 252 Cf funds to purchase additional or upgraded manipulators.

07 ISOTOPE AND RADIATION SOURCES↗

Development of Type A Transport Packagings - 17073a

ORNL ships a wide variety of radioisotopes. Many of these are associated with the DOE Isotope Program and Office of Nuclear Materials Integration (ONMI) and can be shipped as DOT Type A quantities of material. The DOT Specification 6M Type B packaging previously used for many shipments at ORNL is no longer authorized. Most materials could be shipped in Type B packagings, but many of them can meet the requirements for shipping as Type A. As a result, ORNL is working with a packaging manufacturer to develop, test, and certify several Type A packagings. These include a 38 L (10 gal) Type A packaging primarily to be used for transport of Cf-252 sources, a 208 L (55 gal) Type A packaging primarily to be used for transport of americium/curium/lanthanide oxide materials recovered from high-burnup targets, and a Type A packaging for transport of irradiated actinium targets. These are being developed with consideration for both gamma and neutron shielding for contents reading up to 5000 R/h. (authors)

07 ISOTOPE AND RADIATION SOURCES↗