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At least 55 records · Page 3

Comparative scintillation performance of EJ-309, EJ-276, and a novel organic glass

An organic glass scintillator developed by Sandia National Laboratories was characterized in terms of its light output and pulse shape discrimination (PSD) properties and compared to commercial liquid (EJ-309) and plastic (EJ-276) organic scintillators. The electron light output was determined through relative comparison of the 137 Cs Compton edge location. The proton light yield was measured using a double time-of-flight technique at the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory. Using a tunable broad-spectrum neutron source and an array of pulse-shape-discriminating observation scintillators, a continuous measurement of the proton light yield was performed for EJ-309 (200 keV–3.2 MeV), EJ-276 (170 keV–4.9 MeV), and the organic glass (50 keV–20 MeV) . Finally, the PSD properties of the organic glass, EJ-309, and EJ-276 were evaluated using an AmBe source and compared via a figure-of-merit metric. The organic glass exhibited a higher electron light output than both EJ-309 and EJ-276. Its proton light yield and PSD performance were comparable to EJ-309 and superior to that of EJ-276. Finally, with these performance characteristics, the organic glass scintillator is well poised to replace current state-of-the-art PSD-capable scintillators in a range of fast neutron detection applications.

47 OTHER INSTRUMENTATION↗

Expansion of the Fast Neutron Hodoscope at TREAT to Support Fuel Safety Experiments

In 2024 the Fuel Motion Monitoring System (FMMS), or Hodoscope, at the Transient Reactor Test Facility, is being expanded from 96 viewing channels to 192 viewing channels, effectively doubling the FMMS field of view. Here, this increase in capability will allow the FMMS to support larger scale fuel tests, encompassing height-of-core test devices, test devices with multi-pin fuel assemblies, and test devices with recirculating coolant flow. Work supporting the expansion included refurbishing 96 additional proton recoil scintillator (PRS) detectors, doubling the data acquisition system (DAS) installed architecture, improving time synchronization in the DAS, and new research to measure the PRS detector energy-dependent, fast-neutron detection efficiency. In addition, laboratory activities have produced an improved benchtop testing capability for assessing the DAS, time synchronization, and external start triggering, along with an updated capability to scan PRS detectors to develop a preliminary flat-field normalization prior to deployment to TREAT.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Performance of a segmented 6 Li-loaded liquid scintillator detector for the PROSPECT experiment

This study describes the design and performance of a 50 liter, two-segment 6 Li-loaded liquid scintillator detector that was designed and operated as prototype for the PROSPECT (Precision Reactor Oscillation and Spectrum) Experiment. The two-segment detector was constructed according to the design specifications of the experiment. It features low-mass optical separators, an integrated source and optical calibration system, and materials that are compatible with the 6 Li-doped scintillator developed by PROSPECT. We demonstrate a high light collection of 850±20 PE/MeV, an energy resolution of σ = 4.0±0.2% at 1 MeV, and efficient pulse-shape discrimination of low dE/dx (electronic recoil) and high dE/dx (nuclear recoil) energy depositions. An effective scintillation attenuation length of 85±3 cm is measured in each segment. The 0.1% by mass concentration of 6 Li in the scintillator results in a measured neutron capture time of τ = 42.8±0.2 μs. The long-term stability of the scintillator is also discussed. Finally, the detector response meets the criteria necessary for achieving the PROSPECT physics goals and demonstrates features that may find application in fast neutron detection.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Gaussian mixture models as automated particle classifiers for fast neutron detectors

Pulse shape discrimination (PSD) is the task of classifying electronic pulse shapes for different particle types such as gamma rays and fast neutrons interacting in scintillators and read out by photo sensitive detectors. This field has been limited in its adoption of techniques found in the statistical learning community. Methods initially employed in the 1960s for analog electronic circuitry persist in the current PSD literature describing operations performed on digitized pulses, which are amenable to statistical rigor. Despite vast amounts of data collected at low energy levels, traditional PSD methods are unable to discriminate particles below a certain threshold. As such, in this work, Gaussian mixture models (GMMs) are used as a clustering technique for fast neutron detection in the absence of labeled data. GMMs yield improvements spanning the energy spectrum in a desirably efficient, unsupervised fashion. An extension, the Dirichlet Process GMM, provides further flexibility and classification improvement.

97 MATHEMATICS AND COMPUTING↗

Recent developments in plastic scintillators with pulse shape discrimination

The paper reports results of studies conducted to improve scintillation performance of plastic scintillators capable of neutron/gamma pulse-shape discrimination (PSD). Compositional modifications made with the polymer matrix improved physical stability, allowing for increased loads of the primary dye that, in combination with selected secondary dyes, provided enhanced PSD especially important for the lower energy ranges. Additional measurements were made with a newly-introduced PSD plastic EJ-276, that replaces the first commercially produced EJ-299. Comparative studies conducted with the new materials and EJ-309 liquids at large scale (up to 10 cm) show that current plastics may provide scintillation and PSD performance sufficient for the replacement of liquid scintillators. In conclusion, comparison to stilbene single crystals compliments the information about the status of the solid-state materials recently developed for fast neutron detection applications.

36 MATERIALS SCIENCE↗

Light output quenching in response to deuterium-ions and alpha particles and pulse shape discrimination in deuterated trans-stilbene

We characterized the light output response of a new 140 cm 3 stilbene-d 12 crystal up to 14.1 MeV neutron energies using a coincidence neutron scattering system. We also characterized its light output response to alpha particles in the 5 to 6 MeV energy range. The excellent PSD capability of the stilbene-d 12 detector allowed us to select light pulses produced by particles of increasing ionization density, namely electrons, protons, deuterium-ions, and alpha particles. The measured fast decay component of the light pulses is increasingly quenched as the ionization density of the particle in the crystal increases. Consistently with this finding, the Birks’ quenching parameter of alpha particles is approximately 8.5 times larger compared to the quenching of deuterium ions, produced by neutron scattering interactions. The reported experimental characterization will allow high-fidelity modeling of the detector enabling its application for fast-neutron detection and spectroscopy in nuclear physics, radiation protection, nuclear security, and non-proliferation.

36 MATERIALS SCIENCE↗

2018 fourth quarter report to NA-22 on Particle Classifier

This was the final quarter of the third and final year of this project. The team prepared and submitted this project’s final report to NA-22. Work during this quarter included responding to reviewer requests for the unsupervised statistical model paper for the American Statistical Association journal, and completing and submitting the paper about the semi-supervised statistical model to NIMA. We received the report from our North Carolina State University collaborators from the NA-22-sponsored CNEC Consortium, Professor Wilson and student Allen. The report describes their investigation of Dirichlet Process (DP) Gaussian Mixture Models based on pulse shape data from this project. The report is an appendix to this project’s final report, and may be converted into a journal paper in the coming year. Work was performed on the user interface to the Struck firmware. The project team submitted a draft workplan to NA-22 regarding additional work to diffuse improved PSD methods through the NA-22 fast neutron detection community.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Manhattan Project 1940s research on the prompt fission neutron spectrum

We describe how the prompt fission neutron spectrum (PFNS) was determined for the Manhattan Project at Los Alamos. Early work before World War II at American and British universities is described, together with theoretical work by Feather at Cambridge and Bethe at Los Alamos. As the Manhattan Project was being planned in 1942, two experiments on natural uranium were commissioned that proved to be influential: 1) An integral experiment at Chicago by Christy and Manley that accurately determined the average PFNS spectrum energy, 2.2 ± 0.2 MeV; 2) Bloch and Staub’s Stanford cyclotron measurement of the PFNS spectrum, which obtained an average energy of 1.70 ± 0.34 MeV. These two papers, previously unavailable outside of Los Alamos, are reproduced in the Supplementary Appendix. From these data, at the beginning of the project in 1943 Serber estimated an average 235 U PFNS energy of 2 MeV, and indeed this agrees with today’s best estimate. The challenges facing the scientists involved both the availability of only very small samples of enriched uranium and plutonium targets, and fast neutron detection technologies. During the project, 235 U and 239 Pu PFNS were measured by Nicodemus and Staub. These also proved to be quite accurate and gave an average spectrum energy of 2 MeV for 235 U. [This is not reproduced in the Appendix because it was published after the war in Physical Review 89, 1288 (1953)]. New methods were developed to enable more accurate measurements, and this paper describes how the PFNS was determined surprisingly well by 1945. We end by describing the post-war measurements in the 50s, including the PFNS data used by Ford and Wheeler in their simulations in 1951, the Bonner 1952 data, the seminal 1952 Watt paper with a new empirical parametrization of the PFNS, and the accurate PFNS measurement undertaken at Los Alamos by Cranberg et al. in 1956. We compare the measurements with our best understanding today as embodied in the Evaluated Nuclear Data File ENDF/B-VIII.0. Some images from historical documents in our Los Alamos National Security Research Center (NSRC) archives are shown.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗

Characterization of a boron-loaded deuterated liquid scintillator for fast and thermal neutron detection

The preparation and characterization of novel boron-loaded deuterated liquid scintillators (BLDLS) are presented for the first time to investigate the performance of a detector sensitive to both fast and thermal neutrons intended for future neutron spectroscopy measurements. Three deuterated toluene-based scintillation cocktails were produced, one without boron, one loaded with ortho-carborane (natural boron isotopic abundance), and one with 96 wt% 10B enriched ortho-carborane. General optical and material properties were analyzed to include the composition, density, index of refraction, photoluminescence emission spectra, and absorbance spectra in addition to the relative light yield, resolution, relative efficiency, and pulse-shape-discrimination performance for all three scintillators and a hydrogen-based EJ-309 scintillator to evaluate the effects of boron loading in comparison with a common commercially-available scintillator and feasibility for future neutron spectroscopy measurements. Finally, the detection of shielded neutron sources was explored to capitalize on the 10B thermal neutron capture reaction. The results showed loading the scintillators with boron deteriorated the PSD performance slightly compared to the unloaded deuterated scintillator and resulted in a relative light yield loss of 26% and 41% for the 10B enriched and natural boron BLDLS, respectively. Lastly, the BLDLS have a higher relative detection efficiency than the unloaded deuterated scintillator for shielded neutron sources, based on total count rate, a desirable characteristic for missions related to finding and characterizing illicitly-trafficked special nuclear material.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Lithium-containing scintillators for thermal neutron, fast neutron, and gamma detection

In one embodiment, a scintillator includes a scintillator material; a primary fluor, and a Li-containing compound, where the Li-containing compound is soluble in the primary fluor, and where the scintillator exhibits an optical response signature for thermal neutrons that is different than an optical response signature for fast neutrons and gamma rays.

36 MATERIALS SCIENCE↗

Fuel Motion Monitoring System at TREAT – FY2017 Instrumentation Summary

This document is a report summarizing FY2017 efforts related to the Transient Reactor Test Facility (TREAT) Fuel Motion Monitoring System, "hodoscope," refurbishment campaign. TREAT is an air-cooled, graphite-moderated, heterogeneous test facility designed to evaluate reactor fuels and structural materials under conditions that simulate various types of transient overpower and under-cooling situations in a nuclear reactor. Fuel meltdowns, metal-water reactions, thermal interaction between overheated fuel and coolant, and the transient behavior of ceramic fuel for high-temperature systems can be studied. A key instrument that monitors fuel motion as these events take place is the fast neutron hodoscope. The hodoscope is designed to allow for pre-, during-, and post- transient imaging of fuel within a test loop in the center of the reactor core. The preferred technique for imaging is detection of fast neutrons produced by fission in the test fuel, travelling unmoderated through an empty row of core fuel assemblies and then through a multi-slot collimator to a 360-detector array. Due to the age of the instrument, a refurbishment of the hodoscope’s fast neutron detection capability is necessary to support real-time, fuel-position experimental data collection. One particular challenge in this regard is related to the refurbishment of the fast-neutron-sensing detector elements in the detector array. This report summarizes major activities and accomplishments related to the FMMS refurbishment in FY2017. Of particular note was work related to identifying options for new proton recoil scintillator wafer and initial examination of the TREAT proton recoil proportional counter detectors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fast-Neutron Multiplicity Counter for the Detection of Diversion Scenarios

We demonstrated the application of a fast-neutron multiplicity counter (FNMC) to detect small variations in an assembly of uranium-oxide pins. The current version of the FNMC includes eight liquid organic scintillators (EJ-309 7.62 cm diameter x 7.62 cm) and eight crystal organic scintillators (stilbene 5.08 cm diameter x 5.08 cm) in a checkerboard assembly. We measured time-correlated fast neutrons, emitted by an assembly of 32 uranium-oxide pins, using two AmLi sources to induce fissions in the sample. Each pin is a cylinder of approximately 1 cm diameter and 10 cm length, with a mass of 75.52 g and 16.37 wt% enrichment. We removed up to 16 pins from a sample consisting of 32 pins, and determined the minimum number of pins that resulted in a statistically significant decrease of neutron coincidence counts. All the measurements were performed at the Zero Power Physics Reactor facility of Idaho National Laboratory. We found that a diversion of the four innermost pins could be detected by the system in 5 minutes. The detection of time-correlated neutrons requires their discrimination from gamma-ray events. This is an especially challenging task when measuring uranium isotopes, because of the intense gamma-ray flux generated by the radioactive decay of uranium daughters. We will describe the on-board pulse shape discrimination and post processing techniques that we applied to effectively distinguish neutrons from gamma-rays. Fast-neutron measurements have several potential advantages compared to thermal and epithermal neutron counters, the most important being a shorter die-away time and therefore reduced spurious coincidences due to accidental counts. This advantage may result in a higher sensitivity in timely detecting diversion of nuclear material from peaceful uses.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Improvement in the spatial resolution for imaging with fast neutrons

In this paper, we report on the realization of an improved concept for the detection of fast neutrons using a specific setup of scintillators with the aim to overcome limitations in spatial resolution. While fast neutron imaging (FNI) is a technique to investigate very thick material layers in transmission mode, currently there is a limit in the spatial resolution at ~1 mm, which hinders the performance for the detection of features like cracks, material damage or pores in large objects ($\gg$1 cm 3 ). The improved concept presented here is based on the separation of the converter material from the scintillation layer in a suitable way, which was successfully tested and referenced to the standard devices at the NECTAR facility (FRM-2, MLZ, Garching) under realistic beamline conditions. The results imply a break-through in enabling detection of structures on the order of 0.2 to 0.5 mm (a more precise estimation is not possible due to other resolution determing factors in a realistic setup). Potential additional improvements are discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Initial Investigation of the Small Feature Detection Capability of the ORNL Fast Neutron Tomographic Imaging System

A variety of fast neutron imaging simulations and measurements were performed to investigate the spatial resolution and small feature detection capability of a fast-neutron tomographic imaging system developed at Oak Ridge National Laboratory. The system uses an associated particle DT (deuterium-tritium) neutron generator as the source and 25 mm × 25 mm × 100 mm plastic scintillators as the neutron detectors. Two image quality indicators were examined: 1) a variety of long steel pins embedded axially in the interior of a polyethylene cylinder and 2) a variety of short steels pins embedded radially in the surface of a shielded polyethylene cylinder. Measurements demonstrated detectability down to approximately 3 mm. Further data analysis may show improved detection performance and allow a more precise determination of the spatial resolution and small feature detection limit. The current DT generator has a neutron production spot size of about 3.5 mm, which appears to be the limiting factor in the current system configuration.

Wright, Michael C.↗

Initial Investigation of the Small Feature Detection Capability of the ORNL Fast Neutron Tomographic Imaging System

A variety of fast neutron imaging simulations and measurements were performed to investigate the spatial resolution and small feature detection capability of a version of the Oak Ridge National Laboratory fast neutron tomographic imaging system. Two image quality indicators were examined: (1) a variety of long steel pins embedded axially in the interior of a polyethylene cylinder, and (2) a variety of short steels pins embedded radially in the surface of a polyethylene cylinder. Measurements demonstrated detectability of about 3 mm. Further data analysis may show improved detection performance and allow a more precise determination of the spatial resolution. Our current simulation code takes only partial consideration of the DT generator neutron production spot size, with neutron production effectively originating at a single point. Simulations showed that features less than 2 mm should be detectable with an improved generator. Our current ING-27 DT generator has a neutron production spot size of about 3.5 mm, which appears to be the limiting factor at present. Generators with spot sizes as small as 1 mm are commercially available. Higher-power, small–spot size associated particle generators are at the prototype stage and are expected to be commercially available soon.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Used Fuel Storage Monitoring Using Helium-4 Scintillation Fast Neutron Detectors and Neutron Spectral Analysis

This project aimed to address the technology gap in the reliable methods to verify contents of sealed dry storage casks for spent nuclear fuel. Helium-4 gas scintillation neutron detectors was proposed to be developed into a neutron spectroscopy and imaging system for nuclear security and safeguards applications. 4 He gas is significantly more available than 3 He gas and it has unique advantages such as low gamma interaction probability and direct detection of fast neutrons. Due to the sheer amount of fissile materials in a single dry cask, there is a significant neutron fluence emitted whose energies range from thermal to uncollided high-energy neutrons suitable for the detection capability of the 4 He detectors. Our project demonstrated the first ever neutron spectroscopic capabilities using 4 He detectors, explored novel detector design and performed detector characterization. It further qualified the detectors for use in various applications including high-flux environments with significant gamma-fluence. Computer simulations were used to test various large cask measurement system designs and tests, beyond the compact prototype system and laboratory measurements exploring the feasibility of the neutron spectroscopic approach. Although some cask-characterization methods proved unfeasible, alternative characterization methods using the He-4 detectors were explored and generated promising results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Systematic evaluation of fast neutron sensing with Cesium Hafnium Chloride

Cesium Hafnium Chloride (CHC) is a promising new scintillator for dual mode sensing of both neutrons and gamma-rays. The high chlorine content allows for both 35 Cl(n,p) 35 S and 35 Cl(n,α) 32 P reaction channels leading to reliable detection of fast neutrons. By utilizing pulse shape discrimination (PSD), these neutron interactions may be reliably separated from gamma-ray signals with a high figure-of-merit (FOM) after optimization of the PSD algorithm. Here, in this study, the PSD algorithm settings for CHC were systematically investigated using a bare 252 Cf and a lead shielded plutonium beryllium neutron source. It was found that the PSD algorithm settings affects both the FOM and the neutron detection efficiency, but a FOM as high as 4.5 for alpha particles was observed in one data processing scenario. Further, an intrinsic 5 parts per million alpha emitting contamination was observed in the sample, which we attribute to natural uranium.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗