Spatially REsolved Fission Tag (SREFT) - a low-mass TPC
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73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
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Measurement of fragment-correlated γ-ray emission from 252 Cf(sf)
This paper presents recent experimental results on the yield of prompt fission γ rays from the spontaneous fission of 252 Cf. We use an ionization chamber to tag fission events and measure the masses and kinetic energies of the fission fragments and trans-stilbene organic scintillators to measure the neutrons and γ rays emitted by the fission fragments. The combination of the ionization chamber and trans-stilbene scintillators allows us to determine the properties of neutrons and γ rays in coincidence with the fragments. The yield of γ rays is known to be influenced by the angular momenta (AM) of the fission fragments. We present experimental evidence indicating that the total γ-ray multiplicity, i.e., the sum of both fragments' emission, saturates at sufficiently high internal fragment excitation energies. We also observe distinct behaviors for the yield of γ rays from the light and heavy fragments, which for certain mass and total kinetic energy (TKE) regions are weakly or anticorrelated, indicating the presence of complex AM generation modes. We also observed a mass- and TKE-dependent anisotropy of the γ rays, which challenges and expands on the conventional notion that the fragments' AM are always aligned perpendicularly to the fission axis. Furthermore, the dependence of the anisotropy on mass and TKE indicates a dependence of these properties on the specific fission channels, thus providing an insight into the deformations and dynamics in fission and their connection with experimentally observable quantities.
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Precision determination of the 235 U neutron-capture cross section
A precise knowledge of the probability for the 235 U(n,γ) neutron-capture reaction is required for accurate calculations of reactivity and gamma-ray production in fissioning systems. Surprisingly, there are few measurements of neutron capture at neutron energies above 1 keV, and their uncertainties are mostly in the 10% or greater range. The uncertainties of the most precise data in this region, measured by Jandel et al., range from 6% near 10 keV to 10% at 100 keV. We propose to make a new determination of the capture cross section from 1 keV to roughly 100 keV (higher if possible) by extending the analysis of data taken previously using the DANCE gamma ray detector array at the Los Alamos Neutron Scattering Center. Three weeks of data were obtained on a 235 U sample and the associated backgrounds using DANCE and the NEUANCE neutron detector array (for fission tagging). This data was analyzed to measure the probability of exciting isomers in 236 U at 687.5 and 1052 keV excitation by neutron capture, but cross sections were not determined. We propose to extend the analysis of this data to extract the capture cross sections. We will follow the method in ref 1 of normalizing the results to the fission reaction measured simultaneously in the same target, eliminating several sources of systematic uncertainty. The statistical uncertainty of this data set is expected to give cross-section results in the 3 to 5% uncertainty range up to several hundred keV neutron energy. We will investigate the effect of the isomers studied in on the cross sections. In addition, we will analyze the gamma-ray emission spectra and compare them to model calculations to advance our knowledge of the models needed to predict neutron capture and gamma-ray emission.
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Unifying measurement of Pu 239 ( n , γ ) in the keV to MeV energy regime
A single, unifying measurement of the 239 Pu capture cross section from 1 keV to 1.3 MeV has been performed for the first time using the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center (LANSCE). The experimental method combines a prior experiment's characterization of prompt fission γ rays in conjunction with a fission tagging detector with a separate experiment using a thick 239 Pu sample to extract the neutron capture cross section in ratio to 239 Pu (n, f). We have made new predictions of the capture cross section taking into account recent results for the M1 scissors mode present in other actinides. The results show deviations from current evaluations which are 30% higher at the highest energies, and will be used to improve calculations relevant for several applications.
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Measurement of prompt fission neutron spectrum for spontaneous fission of Cf 252 using γ multiplicity tagging
The prompt fission neutron spectrum from spontaneous fission of 252 Cf is an integral part of several aspects of nuclear data. Not only is the spectrum itself of interest, but neutron detectors often use the spectrum for calibration, and other prompt fission neutron spectra are measured as a ratio to 252 Cf. Therefore, reducing the uncertainties in this spectrum will allow for more accurate nuclear data to be available across a wide range of fields. The prompt fission neutron spectrum for the spontaneous fission of 252 Cf was measured at Rensselaer Polytechnic Institute using the multiple γ tagging method with a 18.4-ng fission sample. An EJ-301 liquid scintillator fast neutron detector was used to measure the high energy portion of the spectrum, 0.5–7 MeV, and a thin EJ-204 plastic scintillator was used to measure the low energy portion of the spectrum, from 50 keV to 2 MeV. These spectra both show good agreement with the current evaluation of 252 Cf and have low associated uncertainties providing a new high precision measurement that helps reduce the uncertainties in the prompt fission neutron spectrum for the spontaneous fission of 252 Cf.
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A method to measure prompt fission neutron spectrum using gamma multiplicity tagging
In order to improve on current prompt fission neutron spectrum measurements, a gamma multiplicity tagging method was developed at the Rensselaer Polytechnic Institute Gearttner Linear Accelerator Center. This method involves using a coincidence requirement on an array of BaF 2 gamma detectors to determine the timing of a fission event. This allows for much larger fission samples to be used due to the higher penetrability of gammas compared to fission fragments. Additionally, since the method relies on gammas as opposed to fission fragments, the effects of the low level discriminator, used in fission chambers to eliminate alpha events, are not seen. A 252 Cf fission chamber was constructed in order to determine the viability of this method as well as the efficiency when compared to a fission chamber. The implemented multiple gamma tagging method was found to accurately reproduce the prompt fission neutron spectrum for the spontaneous fission of 252 Cf and to detect 30% of fission events.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Measurement of Fission Neutron Spectrum and Multiplicity using a Gamma Tag Double Time-of-flight Setup
Recent efforts have been made to improve the prompt fission neutron spectrum and nu-bar measurements for Uranium and Plutonium isotopes particularly in the keV region. A system has been designed at Rensselaer Polytechnic Institute (RPI) utilizing an array of EJ-301 liquid scintillators as well as lithium glass and plastic scintillators to experimentally determine these values. An array of BaF2 detectors was recently obtained from Oak Ridge National Laboratory to be used in conjunction with the neutron detectors. The system uses a novel gamma tagging method for fission which can offer an improvement over conventional fission chambers due to increased sample mass. A coincidence requirement on the gamma detectors from prompt fission gammas is used as the fission tag for the system as opposed to fission fragments in a conventional fission chamber. The system utilizes pulse digitization using Acqiris 8 bit digitizer boards which allow for gamma/neutron pulse height discrimination on the liquid scintillators during post processing. Additionally, a 252Cf fission chamber was designed and constructed at RPI which allowed for optimization and testing of the system without the need for an external neutron source. The characteristics of the gamma tagging method such as false detection rate and detection efficiency were determined using this fission chamber and verified using MCNP Polimi modeling. Prompt fission neutron spectrum data has been taken using the fission chamber focusing on the minimum detectable neutron energy for each of the various detectors. Plastic scintillators were found to offer a significant improvement over traditional liquid scintillators allowing energy measurements down to 50 keV. Background was also characterized for all detectors and will be discussed.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Neutron-induced capture-to-fission cross section ratio measured at LANSCE
Capture-to-fission cross section ratios are used as an alternative to absolute cross section measurements. This is due to the simplification on the calculations and the reduction of the uncertainties with respect to an absolute measurement of the cross section by eliminating experimental complications like self-absorption, beam/target overlap and non-uniformities. Different capture-to-fission reactions have been measured through the years at the Los Alamos Neutron Science Center (LANSCE) at Los Alamos National Laboratory (LANL) using the Detector for Advanced Neutron Capture Experiments (DANCE) combined with different fission detectors. Some of these are a Parallel Plate Avalanche Counter (PPAC) to detect fission fragments (FF), and the NEUtron detector array at DANCE (NEUANCE) to detect fission neutrons. As DANCE detects the γ-rays produced in capture and fission reactions, the fission instrument placed inside the DANCE cavity is used to tag the fission γ-rays for background identification and subtraction. Some examples of capture-to-fission ratio measurements performed with DANCE in the last years are the 233 U, 235 U and 239 Pu. The measurement technique, the different setups, and other potential applications of the instruments will be explained.
Nuclear Criticality Safety Program (NCSP)↗
Correlated fission data measurements with DANCE and NEUANCE
To enhance the capabilities of the DANCE array, a new detector array NEUANCE was developed to enable simultaneous measurements of prompt fission neutrons and γ rays. NEUANCE was designed and constructed using 21 stilbene organic scintillator crystals. It was installed in the central cavity of the DANCE array. Signals from the 160 BaF 2 detectors of DANCE and the 21 detectors of NEUANCE were merged into a newly designed high-density high-throughput data acquisition system. The excellent pulse shape discrimination properties of stilbene enabled detection of neutrons with energy thresholds as low as 30–40 keVee. A fission reaction tagging method was developed using a NEUANCE γ-ray or neutron signal. The probability of detecting a neutron from the spontaneous fission of 252 Cf using NEUANCE is 47%. New correlated data for prompt fission neutrons and prompt fission rays were obtained for 252 Cf using this high detection efficiency experimental setup. In conclusion, average properties of prompt fission neutron emission as a function of prompt fission γ-ray quantities were also obtained, suggesting that neutron and γ-ray emission in fission are correlated.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Capture and fission with DANCE and NEUANCE
A summary of the current and future experimental program at DANCE is presented. Measurements of neutron capture cross sections are planned for many actinide isotopes with the goal to reduce the present uncertainties in nuclear data libraries. Detailed studies of capture gamma rays in the neutron resonance region will be performed in order to derive correlated data on the de-excitation of the compound nucleus. New approaches on how to remove the DANCE detector response from experimental data and retain the correlations between the cascade gamma rays are presented. Studies on 235 U are focused on quantifying the population of short-lived isomeric states in 236 U after neutron capture. For this purpose, a new neutron detector array NEUANCE is under construction. It will be installed in the central cavity of the DANCE array and enable the highly efficient tagging of fission and capture events. In addition, developments of fission fragment detectors are also underway to expand DANCE capabilities to measurements of fully correlated data on fission observables.
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233 U(n,$\gamma$) measurements at LANSCE [Slides]
A new measurement at LANSCE combined DANCE and NEUANCE at the end of 2020 and 2021. The 233 U material was provided by Oak Ridge National Laboratory (December 2020).Two samples of 10 mg and 20 mg of 233 U have been prepared at LANL by Evelyn M. Bond (December 2020). The experiment was performed in December 2020 and June/July 2021. Data analysis is ongoing to extract capture data knowing fission. LANL is looking forward to delivering the capture/fission ratio from (1-300) keV by the end of the FY2022.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
233 U(n,$\gamma$) measurements at LANSCE [Slides]
A new measurement at LANSCE combined DANCE and NEUANCE at the end of 2020 and 2021. The 233 U material was provided by Oak Ridge National Laboratory (December 2020).Two samples of 10 mg and 20 mg of 233 U have been prepared at LANL by Evelyn M. Bond (December 2020). The experiment was performed in December 2020 and June/July 2021. Data analysis is ongoing to extract capture data knowing fission. LANL is looking forward to delivering the capture/fission ratio from (1-300) keV by the end of the FY2022.
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Delayed Critical and Subcritical Experiments with Polyethylene Moderated Unreflected Thin 15 in. Diameter HEU Metal Plates
The thin ~15 in. diameter highly enriched uranium (HEU) metal plates were assembled to delayed criticality at the Oak Ridge Critical Experiments Facility (ORCEF) in 1969 with various thicknesses of polyethylene (varying from 1/16 to 2$\frac{3}{8}$ inches) between uranium metal plates. The average 235 U enrichment was 93.27 wt. %. These unreflected critical configurations contained 4$\frac{2}{3}$ to 20$\frac{5}{6}$ thin 15 in. diameter HEU metal plates (on loan from Los Alamos National Laboratory [LANL] and shipped to Oak Ridge National Laboratory [ORNL] on June 3, 1969). Depending on the thickness of polyethylene, the enriched uranium masses varying from 28,053 to 135,148 grams. Fractional plate sections consisted of the appropriate number of 60° pie sections. In addition to the measurement at delayed criticality, subcritical measurements were also performed by the inverse kinetic rod drop method. Prompt neutron decay constant measurements were also performed by the Rossi alpha and randomly pulsed neutron method using a time-tagged spontaneous fission californium neutron source; these are briefly reported here. At the time of these measurements in 1969, the thin HEU metal plates were in near-pristine condition with extremely little oxidation, allowing better descriptions of the uranium plates than the use of these plates in a heavily oxidized and deteriorated condition in recent reflected benchmark experiments at the LANL facility at the Nevada Test Site with these same thin highly enriched uranium metal plates. This report documents the experimental information for the measurements performed so that later researchers can perform the required uncertainty and calculational analyses and documentation to use these data for an International Nuclear Criticality Safety Benchmark Evaluation Program (ICSBEP) or a Nuclear Energy Agency (NEA) benchmark. Data from the experiments described should be acceptable for use as criticality safety benchmark experiments for the ICSBEP and the NEA nuclear criticality safety benchmark program once the uncertainty analysis on the measured neutron multiplication factors is completed. Additional data—such as the dimensional inspection reports, uranium isotopic information, and other relevant particulars—should be retrieved from the Y-12 Plant or LANL and incorporated in the final ICSBEP benchmark. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, the uncertainties in $k_{eff}$ could be as low as ± 0.0002 for some configurations. Other experiments with smaller-diameter than 15 in. diameter HEU metal plates have been benchmarked in HEU-METFAST-001. The prompt neutron time decay measurements could be the basis for an International Reactor Physics Benchmark Program. Preparation of the present report is part of an effort at ORNL to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other US Department of Energy critical experiments facilities using more than 500 operational days of critical facility time. This work for this report publication was supported by the Nuclear Criticality, Radiation Transport and Safety NCSP Program at ORNL.
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Detection Of Special Nuclear Materials Tagged Neutrons
In order to detect Special Nuclear Materials (SNM) in unattended luggage or cargo containers in the field of homeland security, fissions are induced by 14 MeV neutrons produced by an associated particle DT neutron generator, and prompt fission particles correlated with tagged neutron are detected by plastic scintillators. SMN produce high multiplicity events due to induced fissions, whereas nonnuclear materials produce low multiplicity events due to cross-talk, (n,2n) or (n,n'γ) reactions. The data acquisition electronics is made of compact FPGA boards. The coincidence window is triggered by the alpha particle detection, allowing to tag the emission date and direction of the 14 MeV interrogating neutron. The first part of the paper presents experiment vs. calculation comparisons to validate MCNP-PoliMi simulations and the post-processing tools developed with the data analysis framework ROOT. Measurements have been performed using different targets (iron, lead, graphite), first with small plastic scintillators (10 x 10 x 10 cm{sup 3}) and then with large detectors (10 x 10 x 100 cm{sup 3}) to demonstrate that nuclear materials can be differentiated from nonnuclear dense materials (iron, lead) in iron and wood matrixes. A special attention is paid on SNM detection in abandoned luggage. In the second part of the paper, the performances of a cargo container inspection system are studied by numerical simulation, following previous work reported in. Detectors dimensions and shielding against the neutron generator background are optimized for container inspection. Events not correlated to an alpha particle (uncorrelated background), counting statistics, time and energy resolutions of the data acquisition system are all taken into account in a realistic numerical model. The impact of the container matrix (iron, ceramic, wood) has been investigated by studying the system capability to detect a few kilograms of SNM in different positions in the cargo container, within 10 min acquisitions. (authors)
36 MATERIALS SCIENCE↗
Update of CEA DES Criticality-Safety Activities and Perspectives [Slides]
Neutronics staff at CEA DES are in charge of a whole set of modeling and simulation tools for neutronics: nuclear data evaluation and processing, transport codes development, calculation sequences edition, verification, validation and uncertainty analysis. Advanced user groups are in charge of specific nuclear analysis in reactor physics, fuel cycle, criticality-safety, radiation shielding and nuclear instrumentation for CEA and its partners, at all stages of nuclear facilities life cycle. CEA is willing to participate/collaborate on the following issues: detector design, experiments, analysis and evaluation, DH validation by combining TAGS measurements with Fission Yield variance-covariance matrices.
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Characterization of Neutron Emission Rates of Commercial 252 Cf Sources
Accurate knowledge of 252 Cf neutron emission rates is critical for modeling and fast-neutron experiments, yet commercial sources are often supplied without traceable calibration or uncertainty estimates. This report describes a method to characterize 252 Cf sources using a pulse-shape-discrimination (PSD) scintillator. The scintillator was efficiency-calibrated against a time-tagged 252 Cf fission chamber manufactured at ORNL over 40 years ago. Isotopic evolution of the calibration source was modeled using Bateman equations to account for changes in the effective average neutrons per fission at the time of measurement. The calibrated scintillator was then used to measure absolute emission rates of several commercial 252 Cf sources, revealing deviations of up to 12% from nominal manufacturer values. This methodology provides a practical approach for establishing uncertainty-quantified 252 Cf neutron emission rates, improving fidelity in simulations and supporting the accurate interpretation of measurements.
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An Evaluation of Systematic Biases of the Point Kinetics Model for Active Interrogation of Uranium
The point kinetics model relies upon a series of assumptions that simplify the process of neutron fission chain propagation. Tagged neutron interrogation of uranium using 14.1 MeV neutrons can potentially benefit from the use of the point kinetics model, but the appropriateness of the model's assumptions have yet to be validated for this application. The two assumptions considered by this work are the assumption that a single distribution can be used to describe the neutron multiplicity of a chain-starting event and the assumption that parasitic neutron capture within uranium is negligible. Monte Carlo simulations are used to evaluate the appropriateness of each assumption, as well as the consequences on the emitted doubles rate. This work demonstrates that the use of the point kinetics model for this application is possible, but corrections to the source multiplicity assumption are necessary that would likely require prior knowledge of sample isotopics.
Tweardy, Matthew↗
High resolution measurement of tagged two-neutron energy and angle correlations in 252-Cf (sf)
Spontaneous fission events emit prompt neutrons correlated with one another in emission angle and energy. Measurements of these correlations can shed light on the partitioning of the excitation energy between the fragments, even if they are not directly measured. Purpose: We explore the relationship in energy and angle between correlated prompt neutrons emitted from 252 Cf spontaneous fission. Methods: Measurements with the Chi-Nu array provide experimental data for coincident neutrons tagged with a fission chamber signal with 10° angular resolution and 1-ns timing resolution for time-of-flight energy calculations. The experimental results are compared to simulations produced by the fission event generators cgmf, freya, and mcnpx-polimi ipol(1) = 1. Results: We find that the measurements and the simulations all exhibit anisotropic neutron emission, although differences between fission event generators are evident. In conclusion, this work shows that the dependence of detected neutron energy on the energy of another neutron detected in coincidence, although weak, is non-negligible, indicating that there may be correlations in energy between two neutrons emitted in the same fission event..
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