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Development of new Polysiloxane Based Liquid Scintillators

In the last decade, attention toward neutron detection has been growing in the scientific community, driven by new requirements in different fields of application ranging from homeland security to medical and material analysis, from research physics, to nuclear energy production. So far neutron detection, with particular attention to fast neutrons, has been mainly based on organic liquid scintillators, owing to their good efficiency and pulse shape discrimination (PSD) capability. Most of these liquids have however some main drawbacks given by toxicity, flammability, volatility and sensitivity to dissolved oxygen that limits the duration and the quality of their performances with worse handiness and increased costs. Phenyl-substituted polysiloxanes could address most of these issues, being characterized by low toxicity, low volatility and low flammability. Their optical properties can be tailored by changing the phenyl distribution and concentration thus allowing to increase the solubility of organic dyes, to modify the fluorescence spectra and to vary the refractive index of the medium. Furthermore, polysiloxanes have been recently exploited for the production of plastic scintillators with very good chemical and thermal stability and very good radiation hardness and the development of polysiloxane liquid scintillators could allow to combine these interesting properties with the supremacy of liquid scintillators as regarding PSD over plastics. For these reasons, the properties of several phenyl-substituted polysiloxane with different phenyl amounts and different viscosities have been investigated, with particular attention to the scintillation response and the pulse shape discrimination capability, and the results of the investigation are reported in this work. More in details, the scintillation light yield towards gamma rays ({sup 60}Co and {sup 137}Cs) of several polysiloxane liquids has been analyzed and compared with the light yield of a commercial non-toxic liquid scintillator (EJ309). The results have been related to the optical characterization of these materials, especially as regarding the fluorescence response, and the best performing material (1,1,5,5-Tetraphenyl 1,3,3,5-Tetramethyl Trisiloxane) showed a scintillation light-yield only slightly lower than EJ309, proving to be a promising candidate for the production of an efficient polysiloxane based liquid scintillator. The results as regarding the neutron-gamma pulse shape discrimination capability of the best performing materials are also reported in this work and the scintillation decay time of these materials are compared to the results of fluorescence lifetime analysis. PSD tests have been performed at CN accelerator in Legnaro National Laboratories with a 2.2 MeV pulsed neutron beam using TOF procedure and the pulses have been analyzed in order to evidence the PSD capability of every sample. The reported results pave the way to the development of a new promising class of non-toxic liquid scintillating materials for neutron detection, with good light output and interesting PSD characteristics. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Time-resolved fast-neutron radiography of air-water two-phase flows in a rectangular channel by an improved detection system

In a previous work, we have demonstrated the feasibility of high-frame-rate, fast-neutron radiography of generic air-water two-phase flows in a 1.5 cm thick, rectangular flow channel. The experiments have been carried out at the high-intensity, white-beam facility of the Physikalisch-Technische Bundesanstalt, Germany, using an multi-frame, time-resolved detector developed for fast neutron resonance radiography. The results were however not fully optimal and therefore we have decided to modify the detector and optimize it for the given application, which is described in the present work. Furthermore, we managed to improve the image post-processing methodology and the noise suppression. Using the tailored detector and the improved post-processing, significant increase in the image quality and an order of magnitude lower exposure times, down to 3.33 ms, have been achieved with minimized motion artifacts. Similar to the previous study, different two-phase flow regimes such as bubbly slug and churn flows have been examined. The enhanced imaging quality enables an improved prediction of two-phase flow parameters like the instantaneous volumetric gas fraction, bubble size, and bubble velocities. Instantaneous velocity fields around the gas enclosures can also be more robustly predicted using optical flow methods as previously.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Boron-10 Doped Polysiloxanes as Matrix Materials for Application in the Simultaneous Detection and Discrimination of Gamma Rays and Fast and Thermal Neutrons

Three boron-10 enriched aromatic molecules have been synthesized and incorporated into two different commercial polysiloxane resins, Shin Etsu KER-6000 and Wacker SilRes H62-C. Scintillating fluorophores, 9,9-dimethyl-2-phenylfluorene (PhF) and 2,5-diphenyloxazole (PPO), were tested in combination with each resin and boron-10 molecule for the simultaneous detection of gamma rays, fast neutrons, and thermal neutrons. Here, the H62-C resin was able to solubilize a large amount of PhF, in excess of 20 wt%. Cure kinetics were controlled through the addition of divinylbenzene and phenyl tris(dimethylsiloxy)silane cross-linker solution to the H62-C resin, with rheology experiments demonstrating a large reduction in time to gelation when 20 wt% cross-linker solution was added, from more than 4 hours to less than 1 hour. These polysiloxane resins can be cured in 3 hours under air, while common poly(vinyltoluene) scintillators require at least 4 days of heating and oxygen-free conditions. PhF-doped KER-6000 with tolyl boronate pinacol ester exhibited the best overall performance with a light yield of 62% relative to EJ-200 and thermal neutron capture at energies up to 103 keVee (84 keVee for EJ254B-5). Additionally, four samples exhibited light yields surpassing an industry-standard boron-doped plastic scintillator, Eljen’s EJ254B-5. Over the course of ten months, the KER-6000 samples showed precipitation of dopant molecules, which reduced their light yield by 15% on average, while H62-C proved to be more stable with only a 6% reduction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fast Neutron Imaging and Tomography at NIF [Slides]

The presentation at the first Prompt Radiation Detection and Imaging Workshop covered fast neutron and tomography work at the National Ignition Facility (NIF).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Reconstruction of fast neutron direction in segmented organic detectors using deep learning

A method for reconstructing the direction of a fast neutron source using a segmented organic scintillator-based detector and deep learning model is proposed and analyzed. Here, the model is based on recurrent neural network, which can be trained by a sequence of data obtained from an event recorded in the detector and suitably pre-processed. The performance of deep learning-based model is compared with the conventional double-scatter detection algorithm in reconstructing the direction of a fast neutron source. With the deep learning model, the uncertainty in source direction of 0.301 rad is achieved with 100 neutron detection events in a segmented cubic organic scintillator detector with a side length of 46 mm. To reconstruct the source direction with the same angular resolution as the double-scatter algorithm, the deep learning method requires 75% fewer events. Application of this method could augment the operation of segmented detectors operated in the neutron scatter camera configuration for applications such as special nuclear material detection.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

{sup 4}H-SiC neutron sensors based on ion implanted {sup 10}B neutron converter layer

In the framework of the I{sub S}MART project the main aim is to develop an innovative complete radiation detection system based on silicon carbide technology in view to detect neutrons (thermal and fast) and photons for harsh environments. In the present work two geometries have been realized based on ion implantation of boron. In the first geometry, {sup 10}B ions have been implanted into the Al metallic contact to create the neutron converter layer. In the second geometry one single process has been used to realize both the p+-layer and the neutron converter layer. The technological processes followed to fabricate these detectors, with a study of their electrical behavior and their responses under thermal neutron irradiations are addressed in this paper. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

An Artificial Neural Network System for Photon-Based Active Interrogation Applications

Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.

42 ENGINEERING↗

HPGe detector shielding optimization with MCNPX for the MEDINA PGNAA cell

Radioactive waste repositories must guarantee the non-toxicity of the waste in the long term, not only regarding radioactivity but also regarding other environmental contamination such as toxic chemicals. Analytical methods already exist for chemical characterization (ICP-MS, ICP-AES...) but they are based on test sampling. A possible alternative, for waste packages with an appropriate gamma radiation level, is to use Prompt Gamma Neutron Activation Analysis (PGNAA), a non-destructive measurement technique sensitive to several toxic chemicals. In view of the characterization of radioactive wastes in Germany and France, collaboration between the CEA Cadarache (France) and the Forschungszentrum Juelich (Germany) was initiated a few years ago. FZJ holds a PGNAA graphite cell called MEDINA (Multi Element Detection based on Instrumental Neutron Activation), allowing the characterization of 225 L drums. Fast neutrons are emitted from a D-T pulsed 14 MeV neutron generator and thermalized in graphite to induced radiative captures in the waste materials. Prompt capture gamma rays are detected using a 104% relative efficiency n-type HPGe. However, HPGe crystal is sensitive to fast neutron damage and to thermal neutron activation. A thermal neutron shield made of lithium fluorine and lithium carbonate is already used around the detector. In order to further decrease the current of fast and thermal neutrons coming into the crystal without penalizing MEDINA sensitivity (by decreasing the thermal neutron flux and neutron die away time of the cell, the gamma detection efficiency, or increasing the gamma background), some configurations based on easy-to-implement modifications of MEDINA have been simulated with MCNPX with a model of the cell already validated by experiments. Results show that fast and thermal neutron incoming current in the HPGe could easily be reduced by about a factor of 2 by additional quantities of graphite and by replacing lithium carbonate by lithium fluorine with a higher {sup 6}Li concentration. In addition, these modifications slightly increase the thermal neutron flux in the cell without deteriorating the neutron die away time, and reduce the gamma background about a factor of 2 during the neutron pulse but 5 times less after it. More important changes have also been tested, such as the addition of polyethylene and lead between the neutron generator and the HPGe detector, which is more effective regarding neutron shielding but decreases the neutron die away time, partly compensated by a larger initial thermal neutron flux. Concerning gamma background, hydrogen capture gamma ray (2.23 MeV) is increased due to the presence of polyethylene but lead around the HPGe decreases the total gamma background. In conclusion, simple modifications are possible to improve detector shielding and life time before thermal annealing of the crystal, without reducing MEDINA cell performances. Some of these modifications will be tested in the coming months. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The perturbation of backscattered fast neutrons spectrum caused by the resonances of C, N and O for possible use in pyromaterial detection

Neutron radiation is able to determine the signature of land mine detection based on backscattering energy spectrum of landmine. In this study, the Monte Carlo simulation of backscattered fast neutrons was performed on four basic elements of land mine; hydrogen, nitrogen, oxygen and carbon. The moderation of fast neutrons to thermal neutrons and their resonances cross-section between 0.01 eV until 14 MeV were analysed. The neutrons energies were divided into 29 groups and ten million neutrons particles histories were used. The geometries consist of four main components: neutrons source, detectors, landmine and soil. The neutrons source was placed at the origin coordinate and shielded with carbon and polyethylene. Americium/Beryllium neutron source was placed inside lead casing of 1 cm thick and 2.5 cm height. Polyethylene was used to absorb and disperse radiation and was placed outside the lead shield of width 10 cm and height 7 cm. Two detectors were placed between source with distance of 8 cm and radius of 1.9 cm. Detectors of Helium-3 was used for neutron detection as it has high absorption cross section for thermal neutrons. For the anomaly, the physical is in cylinder form with radius of 10 cm and 8.9 cm height. The anomaly is buried 5 cm deep in the bed soil measured 80 cm radius and 53.5 cm height. The results show that the energy spectrum for the four basic elements of landmine with specific pattern which can be used as indication for the presence of landmines.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Pulse shape discrimination of Cs 2 LiYCl 6 :Ce 3+ detectors at high count rate based on triangular and trapezoidal filters

Cs 2 LiYCl 6 :Ce 3+ (CLYC) detectors have demonstrated the capability to simultaneously detect γ-rays and thermal and fast neutrons with medium energy resolution, reasonable detection efficiency, and substantially high pulse shape discrimination performance. In this work, a disadvantage of CLYC detectors is the long scintillation decay times, which causes pulse pile-up at moderate input count rate. Pulse processing algorithms were developed based on triangular and trapezoidal filters to discriminate between neutrons and γ-rays at high count rate. The algorithms were first tested using low-rate data. They exhibit a pulse-shape discrimination performance comparable to that of the charge comparison method, at low rate. Then, they were evaluated at high count rate. Neutrons and γ-rays were adequately identified with high throughput at rates of up to 375 kcps. The algorithm developed using the triangular filter exhibits discrimination capability marginally higher than that of the trapezoidal filter based algorithm irrespective of low or high rate. The algorithms exhibit low computational complexity and are executable on an FPGA in real-time. Finally, they are also suitable for application to other radiation detectors whose pulses are piled-up at high rate owing to long scintillation decay times.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Parametric Evaluation of New Fast Neutron Scintillator Designs

Experiments conducted at Idaho National Laboratory (INL) measured the performance of prototype fast neutron scintillator screens with various scintillator materials deposited in a range of thicknesses on high density polyethylene (HDPE) of varying thickness. The HDPE acts as a converter for the fast neutrons, utilizing a proton recoil reaction to cause the scintillator material to emit photons. INL’s Neutron Radiography (NRAD) Reactor’s North Radiography Station (NRS) beamline has a fast neutron flux (above 1 MeV) greater than 1.5×107 n/cm2s. This study determined which combination of scintillator material and thickness, as well as which HDPE thickness, exhibited the best screen performance for fast neutron imaging based on light output and spatial resolution. The results of these measurements inform development of higher detection quantum efficiency screens for fast neutron imaging.

99 GENERAL AND MISCELLANEOUS↗

A New Safeguards Technique for Spent Fuel Verification in Dry Storage by Using He-4 Detectors - 18262

It is demanded to find key issues and critical paths for verifying and monitoring a spent nuclear fuel cask or storage with a purpose of non-proliferation of nuclear weapon. However, unfortunately there are no reliable methods to verify the containment in a spent nuclear fuel cask or storage. Therefore, research and development (R and D) has been continuously required to develop new and alternative technologies for searching and verifying undeclared nuclear materials, activities, and facilities. Therefore, the present authors have developed a new safeguards technique of passively scanning a spent fuel cask or storage using pressurized He-4 scintillation neutron detectors. A new approach is to quickly verify content in a spent nuclear fuel cask or presence of all special nuclear materials in unknown packages by comparing experimental and computational results. For that, the present authors have developed a new algorithm and user-interface coupled ORIGEN-ARP and MCNP codes, and the prototype safeguards apparatus employing the array of He-4 fast neutron detectors has been designed, built, and tested. The feasibility test of this new apparatus has been performed with Cf-252 neutron sources and the laboratory scale model cask, minimized by a factor of ten compared to the actual dimension of a KN-21 cask. This technique has several advantages over current methods based on neutron and gamma detection; (1) incident neutron energy information is preserved, (2) disturbance of gamma-ray is excellently rejected (discriminated), and (3) much higher neutron counts and operational cost and space-effectiveness are expected since no moderator is required for fast neutrons. The final goal of this study will (1) conduct a prototype instrument and employ it to monitor a nuclear spent fuel cask or storage at a commercial nuclear power reactor facilities, (2) use spectral-specific measurement data to show proof of concept for measurable data successfully converted to quantifiable signatures, such as diversion/removal of fuel, and maintenance of fuel and cask integrity of fuel, and (3) develop a cask imaging capability. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Systematic measurement of fast neutron background fluctuations in an urban area using a mobile detection system

Neutron background measurements using a mobile trailer-based system were conducted in Knoxville, Tennessee. The 0.5 m 2 system consisting of 8 EJ-301 liquid scintillation detectors was used to collect neutron background measurements in order to better understand the systematic background variations that depend solely on the street-level measurement position in a local, downtown area. Data was collected along 5 different streets in the downtown Knoxville area, and the measurements were found to be repeatable. Using 10-min measurements, fractional uncertainty in each measured data point was <2%. Compared with fast neutron background count rates measured away from downtown Knoxville, a reduction in background count rates ranging from 10-50% was observed in the downtown area, sometimes varying substantially over distances of tens of meters. These reductions are attributed to the shielding of adjacent buildings, quantified in part here by the metric angle-of-open-sky. The adjacent buildings may serve to shield cosmic ray neutron flux.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Report on Field Test at INL Cask Farm of Single Detector Fast Neutron Spent Fuel Cask Verification System

Detecting diversion of spent fuel elements in dry storage casks is challenging due to the thick shielding used in cask construction. Measurements on top of the cask to map the underlying arrangement of the fuel elements and looking for anomalous changes over time has proven difficult to achieve using gamma rays due to the high scattering and attenuation from the thick steel structure, weakening information on the present or absence of fuel bundles. Simulations and laboratory experiments suggest that the high-energy neutron flux (>200 keV) measured directly above each fuel bundle is sufficient to produce a position map that enables detection of the present or absence of fuel bundles, and therefore diversion of a spent fuel bundle. A single-detector spent-fuel monitoring technique based on this principle was development at the Lawrence Livermore National Laboratory (LLNL). The INL Cask Farm in the INTEC technical area at Idaho National Laboratory (INL) offers the capability to test this technique on an MC-10 storage cask which has a distribution of full and empty fuel positions. An experimental test plan for the single-detector verification system was developed in consultation with INL personnel to be completed in FY2021. Due to travel advisories related to COVID-19, the experimental test plan was adapted to enable INL personnel to carry out the measurements in consultation with LLNL personnel following shipment of the LLNL system to INL. Field test measurements of the single detector verification system were successfully carried out at the INL cask farm on September 7-9, 2021. This document summarizes results of the field test.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigation of Misuse Potential and Detection for Homogeneous Fluoride Fast Molten Salt Reactors Based on Neutronics Signatures

The International Atomic Energy Agency (IAEA) has obligations to apply safeguards to nuclear material and facilities within States subject to IAEA safeguards agreements. As a result of these obligations, safeguards will need to be applied to Generation IV reactors, including liquid fueled molten salt reactors (MSRs), if they are deployed in States with safeguards agreements. Recently, the IAEA has noted that a growing number of Member States are showing interest in MSR technology. This has been accompanied by an increase in short term development and deployment activities relating to MSRs. To ensure MSRs can be safeguarded effectively and efficiently upon possible future deployment, safeguards approaches and techniques need to be investigated now.

DeGuire, Thomas↗

Gallium oxide (Ga 2 O 3 ) energy dependent scintillation response to fast neutrons and flash gamma-rays

Gallium oxide is a newly emerged ultrawide bandgap (4.9 eV) semiconductor that is suitable as a combined electronics and radiation detection platform. We have experimentally demonstrated fast neutron and gamma-ray scintillation from Czochralski-grown β-Ga 2 O 3 in a recent series (October 2023) of experiments at the unmoderated pulsed neutron spallation source located at the Los Alamos Neutron Science Center. Using the neutron time-of-flight (TOF) technique and a fast-gated intensified CCD camera, we observed energy-dependent neutron scintillation for neutron energies ranging from 1 to 400 MeV, including the 14.1 MeV neutron energy relevant to D–T fusion. Neutron flux is quantified and calibrated by cascading the scintillator after the fission chamber, enabling a detailed analysis of temporal and energy-dependent characteristics of the scintillation events. Further, a pronounced scintillation signal from the spallation gamma flash with a temporal full width of half maximum of ~4 ns is indicative of the material’s rapid response. Neutron energy dependent scintillation is observed using the TOF method at a 22.6-m distance from the neutron source. These results highlight the possibility of developing a Ga 2 O 3 based fusion neutron diagnostic platform integrated with both scintillation and electronics functions on the integrated chip scale.

47 OTHER INSTRUMENTATION↗

Associated particle technique in single-sided geometry for detection of explosives

Associated particle technique (APT) for detection of explosives is well established but has been implemented mostly for fixed portal systems. In certain situations, a portable system is required where the suspect object cannot be moved from site. This paper discusses the development of a portable APT system in single-sided geometry which can be transported to site and requires only one-sided access to the object. The system comprised D-T neutron source and bismuth germanate (BGO) detectors fixed on a portable module. Different aspects of the system have been discussed such as background contribution, time selection, and elemental signatures. The system was used to detect benign samples and explosive simulants under laboratory condition. The elemental ratios obtained by analyzing the gamma spectra show good match with the theoretical ratios.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Identifying Neutron Irradiation in Space to Mitigate Bio-Medical Effects

Ubiquitous GCR high energy particles >1 GeV is primary concern • Medical effects compounded by ionizing dose of radiation from energetic particles- cancer, mutations, microbiome changes • Cancer induction and effects are irreversible after initiation • Long term space radiation exposure is cancer promoting but reversible Secondary GCR and Solar induced neutron spallation is a concern • Produced by interactions with space craft materials, EVA and planetary surfaces • Neutron Quality Factor is 10x that of beta, x-ray or gamma rays Space isn’t friendly to life or electronics! Real-time charged particle and EARLY neutron detection are required. Traveling fast or digging deep are the best protection. Nuclear space propulsion through LENR/LCF/Solid-State Fusion is a good bet!

space medicine↗