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Impact of temperature on light yield and pulse shape discrimination of polysiloxane-based organic scintillators formulated with commercial resins

This work investigates how increased temperature affects neutron/ discrimination and light yield (LY) in several different polysiloxane-based scintillators doped with either 9,9-dimethyl-2-phenylflourene (PhF) or 2,5-diphenyloxazole (PPO) as a primary fluorophore and 9,9-dimethyl-2,7-di((E)-styryl) fluorene (SFS) as the secondary fluorophore. The polysiloxane matrices were prepared from the commercial resins Wacker Lumisil 579 or Shin-Etsu KER-6000. Control scintillators were prepared from poly(vinyltoluene) (PVT), the industry standard matrix, as a reference point for LY and pulse shape discrimination (PSD) measurements. Samples with PhF and PPO dopant concentrations of 1 wt% and 5 wt% in the polysiloxanes and 3 wt% and 5 wt% in the PVT samples were tested at 20 °C, 35 °C, and 50 °C. In the polysiloxane samples, the KER-6000 resin outperformed the Wacker 579 and PhF proved to be a better dopant than PPO in both LY and PSD capabilities. Polysiloxane scintillators showed slight decreases in LY and increases in neutron/discrimination at increased temperatures, while PVT scintillators showed a similar LY decrease with little to no improvement in neutron/discrimination at increased temperatures. Altogether, polysiloxane scintillators may not require recalibration in applications where temperatures increase up to 50 °C.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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 ↗

Thermal Characterization of Tl 2 LiYCl 6 :Ce (TLYC)

Tl 2 LiYCl 6 :Ce (TLYC) is a new dual-detection elpasolite scintillator that can detect and distinguish between gamma rays and neutrons using pulse shape discrimination (PSD). It has a higher density and Z -number than the more mature and well-known elpasolite Cs 2 LiYCl 6 :Ce (CLYC), causing it to have a significantly better gamma-ray stopping power. These properties make TLYC an attractive alternative to CLYC for resource-constrained applications where size and weight are important, such as space or national security applications. Such applications may be subjected to a wide range of temperatures, and therefore, TLYC's performance was characterized for the first time over a temperature range of -20 °C to +50 °C in 10 °C increments. TLYC's thermal response effects on light-output linearity with energy, gamma-ray photopeak energy resolution, detected neutron energy, pulse shapes, and figure of merit (FOM) is analyzed and reported. The light output of TLYC was found to be linear with energy over the tested temperature range and was observed to decrease with increasing temperature. The decay time of the scintillation light output was observed to decrease with decreasing temperature at short times, leading to a decreasing PSD FOM. The gamma-ray photopeak energy resolution was also observed to degrade with decreasing temperature, due to an asymmetric broadening of the photopeak at low temperatures.

36 MATERIALS SCIENCE↗

Comparative analysis of new crystal and plastic scintillators for fast and thermal neutron detection

This paper considers scintillation and physical properties of efficient organic scintillators tested as single crystals and as components of plastics with pulse shape discrimination (PSD). For the first time, single crystals of 9,9-dimethyl-2-phenyl-9H-fluorene (PhF) were grown for studies of the basic scintillation properties of this new compound. Comparison to classical organic crystals, like anthracene, trans-stilbene, and p-terphenyl, and to more recently introduced organic glass showed that the new crystal belongs to a group of the most efficient scintillators, with light output exceeding that of trans-stilbene and PSD comparable to that of p-terphenyl. Furthermore, additional studies were conducted to evaluate scintillation performance and physical properties, like hardness and dye leaching, of plastic scintillators prepared with PhF, organic glass, and liquid diisopropylnaphthalene (DIPN) that were considered as examples for potential replacement of PPO (2,5-diphenyloxazole) in current commercial PSD plastic scintillators. Comparison of the highest performing plastic scintillators prepared with these dyes shows that PhF formulations produced a record light output (LO) increase of 69 % relative to EJ-200. Similar improvements obtained with 6 Li-loaded formulations showed that future development of PSD plastics should not be limited to use of PPO but must involve the search and exploration of new efficient dyes that may lead to discovery of much brighter organic scintillators with improved physical properties required for fast and thermal neutron detection, fast neutron spectroscopy, and antineutrino detection applications.

9,9-dimethyl-2-phenyl-9H-fluorene↗

Multiple dye interactions in plastic scintillators: Effects on pulse shape discrimination

The scintillation process in plastic scintillators has been studied with mixed systems containing high concentrations of multiple fluorescence dyes. It has been shown that the triplet–triplet interaction phenomena leading to the production of delayed light and pulse shape discrimination (PSD) can vary depending on the triplet energies of the interacting dyes. At small differences between the first excited triplet state energies, found to be below 0.1 eV, a pair of interacting dyes of different molecular species can be involved in heterogeneous excitation migration and triplet–triplet annihilation that result in the enhancement of delayed light and PSD, due to the engagement of both dyes in the process. At differences above 0.27 eV, excitation trapping on the lower energy triplet molecules leads to conditions when triplet–triplet migration and annihilation can proceed only homogeneously between molecules of the same species. The results explain the different effects produced by the selection of fluorescent dyes in previously reported PSD systems containing one primary and one secondary dyes. They also demonstrate a non-traditional approach to the design of new plastic scintillators with multiple dyes that, at improved scintillation and PSD performance, may simplify the production process.

36 MATERIALS SCIENCE↗

Boron-loaded organic glass scintillators

Herein we report the progress towards an organic glass scintillator with fast and thermal neutron sensitivity providing “triple” pulse shape discrimination (PSD) through the inclusion of a boron-incorporated aromatic molecule. Here, the commercially available molecule 2-(p-tolyl)-1,3,2-dioxaborinane (TDB) can be readily synthesized in one step using inexpensive materials and incorporated into the organic glass scintillator at 20% by weight or 0.25% 10 B by mass. In addition, we demonstrate that TDB can be easily scaled up and formulated into organic glass scintillator samples to produce a thermal neutron capture signal with a light yield equivalent to 120.4 ± 3.7 keVee, which is the highest value reported in the literature to date.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Generalized method for the optimization of pulse shape discrimination parameters

Organic scintillators exhibit fast timing, high detection efficiency for fast neutrons and pulse shape discrimination (PSD) capability. PSD is essential in mixed radiation fields, where different types of radiation need to be detected and discriminated. In neutron measurements for nuclear security and non proliferation effective PSD is crucial, because a weak neutron signature needs to be detected in the presence of a strong gamma-ray background. Here, the most commonly used deterministic PSD technique is charge integration (CI). This method requires the optimization of specific parameters to obtain the best gamma-neutron separation. These parameters depend on the scintillating material and light readout device and typically require a lengthy optimization process and a calibration reference measurement with a mixed source. In this paper, we propose a new method based on the scintillation fluorescence physics that enables to find the optimum PSD integration gates using only a gamma-ray emitter. We demonstrate our method using three organic scintillation detectors: deuterated trans-stilbene, small-molecule organic glass, and EJ-309. In all the investigated cases, our method allowed finding the optimum PSD CI parameters without the need of iterative optimization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Studies in pulse shape discrimination for an optimized ASIC design

The continued advancements of Silicon Photomultipliers (SiPMs) have made them viable photosensors for low recoil energy Pulse Shape Discrimination (PSD) between fast neutron and gamma interactions when coupled to an appropriate scintillator. At the same time, the large number of channels in a typical array calls for the development of low-cost and low-power electronics. A custom integrated circuit (ASIC) is an ideal solution for this purpose. To assess the requirements for such an ASIC, studies were performed using two scintillators, Stilbene and EJ-276, coupled to a 6 x 6 mm SiPM from Onsemi. We demonstrate that both scintillators are viable for performing PSD for interaction energies from 100 keV to several MeV while optimizing the integration periods used in the PSD metric. These measurements inform the design parameters of the ASIC under development.

Si-PMTs↗

Pulse Shape Discrimination in JSNS 2

JSNS 2 (J-PARC Sterile Neutrino Search at J-PARC Spallation Neutron Source) is an experiment that is searching for sterile neutrinos via the observation of $\overline{ν}$ μ → $\overline{ν}$ e appearance oscillations using neutrinos from muon decay-at-rest. For this search, rejecting cosmic-ray-induced neutron events by Pulse Shape Discrimination (PSD) is essential because the JSNS2 detector is located above ground, on the third floor of the building. We have achieved 94.95% ± 0.15% rejection of neutron events while keeping 92.82% ± 1.77% of signal, electron-like events using a data-driven likelihood method. This article will report the PSD technique using the full fiducial volume of the JSNS2 detector.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Pulse shape discrimination technique for diffuse supernova neutrino background search with JUNO

Pulse shape discrimination (PSD) is widely used in particle and nuclear physics. Specifically in liquid scintillator detectors, PSD facilitates the classification of different particle types based on their energy deposition patterns. This technique is particularly valuable for studies of the diffuse supernova neutrino background (DSNB), nucleon decay, and dark matter searches. This paper presents a detailed investigation of the PSD technique, applied in the DSNB search performed with the Jiangmen Underground Neutrino Observatory (JUNO). Instead of using conventional cut-and-count methods, we employ methods based on boosted decision trees and neural networks and compare their capability to distinguish the DSNB signals from the atmospheric neutrino neutral-current background events. The two methods demonstrate comparable performance, resulting in a 50–80% improvement in signal efficiency compared to a previous study performed for JUNO (An et al. [JUNO] in J Phys G 43(3):030401, 2016). Moreover, we study the dependence of the PSD performance on the visible energy and final state composition of the events and find a significant dependence on the presence/absence of 11 C. Finally, we evaluate the impact of the detector effects (photon propagation, PMT dark noise, and waveform reconstruction) on the PSD performance.

FOS: Physical sciences↗

Replacing photomultiplier tubes with silicon photomultipliers for nuclear safeguards applications

Photomultiplier tubes (PMTs) have been used for decades as the default light detection technology for scintillator-based radiation monitors. PMTs come with a handful of disadvantages, however, including large volume usage, fragility, high-voltage requirements, and susceptibility to magnetic fields. Arrays of silicon photomultipliers (SiPMs) are a possible alternative to PMTs providing similar performance while offering improvements in the areas listed. We focus on straightforward “drop-in replacement” evaluations by imposing a single channel output of the SiPM signal and a backend electronics data acquisition and analysis routine identical to that used for PMTs. In the realm of nuclear safeguards, the primary performance metric for gamma spectroscopy is detector resolution, and for neutron detection it is pulse shape discrimination (PSD) to separate neutron and gamma signals. In this work we present the results of replacing a PMT with a 2” x 2” SiPM array mounted, in turn, to the same 2” x 2” cylindrical sodium iodide (NaI) crystal. The ultimate comparison for this gamma spectrometry is confirmation of uranium enrichment standards, ranging from depleted uranium to 93% highly enriched uranium (HEU), by analyzing the resulting spectra with both a simple integral scaling in key energy regions of the spectrum, as well as with the NaIGEM software package. In addition to the gamma spectroscopy work, we will present the latest results on comparing the PSD capabilities of a 4” x 4” SiPM array to a 5” PMT. As with the gamma spectroscopy evaluations, the light detectors are mounted in turn to the same liter-scale organic scintillators. This neutron-focused work includes evaluation of prototype SiPM readout boards with a single output signal summed over 256 individual SiPM pixels, and evident tradeoffs between PSD capability and fast response.

42 ENGINEERING↗

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.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Passive Confirmation of the Presence Of High-Explosive Material Via Neutron Transmission Spectroscopy

The goal of this project was to explore a novel approach for identifying presence and potential types of high explosives (HE) in treaty-controlled items with passive neutron sources by using passive neutron transmission spectroscopy. We predominantly look to measure relative elemental abundance of Carbon, Hydrogen, Oxygen, and Nitrogen (CHON) since most relevant materials are certain mix of these elements, as shown in Table 1. Previously, most studies exploring potential identification of CHON elemental content of targets in the vicinity of passive neutron source were focused solely on gamma spectroscopy using high resolution gamma detectors. Using neutron transmission spectroscopy with pulse-shape discrimination (PSD) capable organic scintillators is not only a novel idea in of itself, but arguably necessary for accurate identification of the CHON elemental content of an interrogated target. While high resolution gamma spectroscopy in principle can determine a presence of hydrogen and nitrogen, it is effectively blind to a quantitatively measuring areal densities of C, O. The initially proposed approach, described in detail in the project proposal, was to leverage previous Monte Carlo study on neutron transmission spectroscopy using slab shaped target interrogated with well-collimated (“pencil”) neutron beam. In this study, a simulated test CO 2 target was interrogated by a pencil neutron beam and transmitted neutron spectra were measured using PSD capable organic scintillator using MLEM based unfolding technique. To establish relative elemental content of carbon and oxygen, the unfolded neutron spectrum was fit with a parametrized combination of their respective elemental spectral templates. The individual spectral template was calculated by convoluting ENDF neutron crosssection with the known resolution of the PSD detector used in the study. This approach in the studied configuration successfully quantitatively established relative elemental composition of carbon and oxygen.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Deuterated Xylene-Based Neutron Spectrometry

Deuterated scintillators, such as deuterated xylene (C8D10) have been theorized to offer better pulse shape discrimination (PSD) and neutron spectrometry performance than traditional protiated scintillators due to the anisotropy of neutron scattering on deuterium. However, the light output responses of said deuterated scintillators to monoenergetic has not been characterized in its entirety at both high and low energies. Several time-of-flight experiments were conducted at the Idaho national Laboratory to characterize a pair of EJ-301D deuterated xylene detectors. The low energy detector response to quasi-monoenergetic neutrons was measured using a Cf-252 source, and the high energy detector response was measured using a D-T source and angles of 20, 45, and 60 deg, corresponding to theoretical neutron energies of 13.2, 10.4, and 8.2 MeV. During post-processing, the neutron and gamma bands were clearly able to be separated, even at low light outputs, solidifying the superior PSD capability of deuterated xylene. An exponential of fit of LO=0.63E-2.22*(1-exp(-0.25E)), which has good agreement with previously measured data, was found as the light output response from deuteron recoils. Additionally, measurements of AmBe, D-T, and D-D sources were unfolded using the light output response curve, which resulted in favorable agreement with theoretical values. Further testing of the response matrix by unfolding more sources (such as PuBe) needs to be done, but the unfolding accuracy for currently available sources suggests that deuterated xylene can be used to measure and unfold both fission, monoenergetic, and continuous spectra.

scintillator↗

Fast-, Light-Cured Scintillating Plastic for 3D-Printing Applications

Additive manufacturing techniques enable a wide range of possibilities for novel radiation detectors spanning simple to highly complex geometries, multi-material composites, and metamaterials that are either impossible or cost prohibitive to produce using conventional methods. The present work identifies a set of promising formulations of photocurable scintillator resins capable of neutron-gamma pulse shape discrimination (PSD) to support the additive manufacturing of fast neutron detectors. The development of these resins utilizes a step-by-step, trial-and-error approach to identify different monomer and cross-linker combinations that meet the requirements for 3D printing followed by a 2-level factorial parameter study to optimize the radiation detection performance, including light yield, PSD, optical clarity, and hardness. The formulations resulted in hard, clear, PSD-capable plastic scintillators that were cured solid within 10 s using 405 nm light. The best-performing scintillator produced a light yield 83% of EJ-276 and a PSD figure of merit equaling 1.28 at 450–550 keVee.

Frandsen, Brian G. (ORCID:0000000319964320)↗

Replacing photomultiplier tubes with silicon photomultipliers for nuclear safeguards applications

Photomultiplier tubes (PMTs) have been used for decades as the default light detection technology for scintillator-based radiation monitors. PMTs come with a handful of disadvantages, however, including large volume usage, fragility, high-voltage requirements, and susceptibility to magnetic fields. Arrays of silicon photomultipliers (SiPMs) are a possible alternative to PMTs providing similar performance while offering improvements in the areas listed. We focus on straightforward “drop-in replacement” evaluations by imposing a single channel output of the SiPM signal and a backend electronics data acquisition and analysis routine identical to that used for PMTs. In the realm of nuclear safeguards, the primary performance metric for gamma spectroscopy is detector resolution, and for neutron detection it is pulse shape discrimination (PSD) to separate neutron and gamma signals. In this work we present the results of replacing a PMT with a 2” x 2” SiPM array mounted, in turn, to the same 2” x 2” cylindrical sodium iodide (NaI) crystal. The ultimate comparison for this gamma spectrometry is confirmation of uranium enrichment standards, ranging from depleted uranium to 93% highly enriched uranium (HEU), by analyzing the resulting spectra with both a simple integral scaling in key energy regions of the spectrum, as well as with the NaIGEM software package. In addition to the gamma spectroscopy work, we will present the latest results on comparing the PSD capabilities of a 4” x 4” SiPM array to a 5” PMT. As with the gamma spectroscopy evaluations, the light detectors are mounted in turn to the same liter-scale organic scintillators. This neutron-focused work includes evaluation of prototype SiPM readout boards with a single output signal summed over 256 individual SiPM pixels, and evident tradeoffs between PSD capability and fast response.

Engineering - Instrumentation related to nuclear s↗

From Detector Layout to Signal Analysis: Geometry Optimization and Neutron-Gamma Tagging in Plastic Scintillator Detectors

Neutrinos are elementary particles with many properties still unknown. Their masses so far have only upper and lower limits. Still, due to neutrino oscillations, it is clear that they are not massless, as stated by the Standard Model of Elementary Particles. Neutrinos are also present in the Universe in vast amounts, but they rarely interact with the surrounding matter. Their abundance makes them very interesting for many theories beyond the Standard Model, e.g., dark matter searches and CP symmetry violation in the leptonic sector, which could be (partially) responsible for the observed matter-antimatter asymmetry in today's Universe.\\ The Deep Underground Neutrino Experiment (DUNE) is a next-generation accelerator-based neutrino oscillation experiment that will study neutrinos with unprecedented precision and may answer many open questions. DUNE uses a powerful neutrino beam from Fermilab. It consists of a Near Detector (ND) complex to measure neutrinos before oscillat ion, and a Far Detector (FD) complex $1300\ \mathrm{km}$ away to measure them after oscillation. As part of the ND complex, measurements are also possible with different angles to the neutrino beam. This enables excellent control of systematic uncertainties of e.g., neutrino cross section measurements.\\ One detector in the near detector complex is The Muon Spectrometer (TMS), an extension of a Liquid Argon (LAr) detector that measures the charge and momentum of muons produced in neutrino interactions within the LAr. The design of this detector, which consists of alternating layers of steel and plastic scintillator bars, must be optimized for the expected muon energies.\\ In this thesis, a study of the optimal module orientation plan is presented, which is necessary for the physics performance of the near detector complex and, by extension, DUNE. As part of this study, the event reconstruction was also developed and improved. Simulated muons are then reconstructed, and the performan ce of different module orientation plans is tested.\\ As a second part, a study of neutron and gamma tagging using a Pulse Shape Discriminating (PSD) plastic scintillator is presented. The properties of this material allow particle differentiation based on the temporal distribution of emitted light. A novel approach to using the individual light signals was successfully tested using data from a small, local test setup.

Nehm, Asa [Mainz U.]↗