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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↗

On optical properties and scintillation performance of emerging Ga 2 O 3 : Crystal growth, emission mechanisms and doping strategies

As an emerging ultra-wide bandgap compound semiconductor, Ga 2 O 3 has attracted rapidly growing interest due to its unique physical properties for harsh condition applications. Compared to Ga 2 O 3 ’s electrical-characteristic based uses, such as power electronics, photodetectors and solar cells, a much less explored area for Ga 2 O 3 is its promising optical properties and its related scintillation capabilities. Undoped Ga 2 O 3 is a strong scintillator with excellent scintillation characteristics such as fast decay constants and encouraging light yield which is comparable to that of the classic Bi 4 Ge 3 O 12 (BGO) scintillator. The scintillation capability of Ga 2 O 3 can be precisely tuned via a series of approaches including systematic crystal growth control, post-growth annealing, targeted doping, and optimization of operation temperature. Here we summarize exciting progress of Ga 2 O 3 scintillators which have been pursued over the past few years. Our efforts cover a series of growth techniques of Ga 2 O 3 materials as well as discussion of emission mechanisms. Here we dedicate a targeted portion toward the doping strategies to improve the performance of Ga 2 O 3 . A detailed analysis is provided to compare the impact of different dopants. Through these efforts, we hope to provide useful perspectives to help accelerate the development of high performance Ga 2 O 3 scintillators.

36 MATERIALS SCIENCE↗

Synthesis and processing of lithium-loaded plastic scintillators on the kilogram scale

Plastic scintillators that can discriminate between gamma rays, fast neutrons, and thermal neutrons were synthesized and characterized while considering the performance at the kilogram scale. The synthesis and processing of these plastic scintillators on the kilogram scale required examination of several factors. The examination of these factors was necessitated by the inclusion of 0.1 wt.% lithium-6 to enable detection of thermal neutrons. First, methacrylic acid was used as an additive to solubilize salts of lithium-6, which allow for a thermal-neutron capture reaction that produces scintillation light following energy transfer. Second, a trade-off between scintillation performance and processability was considered because the increasing content of the methacrylic acid that aided processability resulted in a sharp decrease in the light output. The use of small amounts of methacrylic acid (≤3 wt.%) resulted in better performance but required high processing temperatures. At large scales, these high temperatures could initiate exothermic polymerization that results in premature curing and/or defects. Additionally, the deleterious effects of the methacrylic acid may be mitigated by using m-terphenyl as a primary dye rather than 2,5-diphenyloxazole (PPO), which has been traditionally used in organic scintillators. Finally, the curing environment was controlled to avoid defects like cracking and discolouration​ while maintaining solubility of dopants during curing. For scintillators that were produced from kilogram-scale batches of precursors, the effective attenuation of scintillation light was characterized.

36 MATERIALS SCIENCE↗

Crystal Growth Scale-Up and Stability of RbSr 2 X 5 :Eu Scintillators

The discovery and development of new scintillation materials support national security needs. In these applications, large volumes of scintillator crystals are needed to achieve efficient screening for contraband. Therefore, one important step in the discovery of new scintillator compositions is testing their feasibility for scale-up and their stability. In this work, high-quality Ø22 mm crystals of two new scintillators RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu were grown via the Vertical Bridgman method, and their scintillation properties were characterized. Here, the Ø22 mm RbSr 2 I 5 :Eu crystals could be grown with fast translation rates up to 3.5 mm/h. Both RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu had high scintillation performance, including light yields of 46,000 and 61,000 ph/MeV, respectively, for Ø22 × 35 mm crystals. Additionally, properties related to physical stability were investigated, including the coefficients of thermal expansion via high-temperature X-ray diffraction (HTXRD) as well as moisture sensitivity. HTXRD confirmed the absence of solid–solid phase transitions and showed that RbSr 2 Br 5 had minimal thermal expansion anisotropy compared to RbSr 2 I 5 and some other inorganic metal halide scintillators, which favors the growth of large-sized crystals.

36 MATERIALS SCIENCE↗

Vertically Self-Oriented, Ultrafast 1D ZnO:Li Nanorods as Scintillators for Thermal Neutron Detection

Detection of special nuclear materials (SNMs) is of vital importance in the prevention of nuclear terrorism and to secure states’ national security. Neutron detection is a particularly useful tool to identify SNM, and neutron-sensitive scintillators have many promising properties, such as ease of use, good time resolution, and high detection efficiency. In this work, we develop highly stable, self-oriented, ultrafast 1D ZnO:Li (and codoped with Al, Ga, and In) nanorods (NRs) as thermal neutron-sensitive scintillators. Lithium-6 has high thermal neutron cross section for the (n, α) reaction in ZnO:Li scintillators which have a vertical nano array design greatly increasing the effective surface area and scintillation efficiency. Cost-effective low-temperature (95 °C) hydrothermal growth is used to obtain highly crystalline ZnO:Li nano scintillators by combining nuclear range data and electron transport mechanisms. Among the studies using low-temperature hydrothermal synthesis and a relatively low annealing temperature (≈350 °C) along with optimized NRs (length ≈ 5–8 μm, mean diameter ≈ 700 nm) for thermal neutron detection, this study reports the shortest scintillation decay time (≈ 470 ps) so far to the best of our knowledge. In conclusion, this nano array scintillator combines the advantages of a low-cost growth technique with environmentally friendly and widely available materials.

Ions↗

Polysiloxane Scintillators for Efficient Neutron and Gamma-Ray Pulse Shape Discrimination

Plastic scintillators based on thermoplastics, such as polystyrene and poly(vinyl toluene) (PVT), are capable of neutron and γ radiation detection via pulse shape discrimination (PSD) when overdoped with select fluorescent molecules. This class of plastic scintillator has been extensively studied but is limited to applications suitable for thermoplastics. For applications requiring flexibility, scintillators composed of elastomers, such as polysiloxanes, offer an alternative to PVT scintillators. Polysiloxane scintillators are inherently flexible and have a short processing time on the order of 3 h in air and equivalent or better detection capability at reduced doping concentration (<5 wt %). This work presents polysiloxane-based scintillators, containing only 1–5 wt % of 2,5 diphenyl-oxazole (PPO) or 9,9-dimethyl-2-phenyl-9H-fluorene (PhF) as primary dopants and 9,9-dimethyl-2,7-distyryl-9H-fluorene (SFS) as a wavelength shifter. A 5 wt % PPO polysiloxane sample had improved neutron and gamma ray PSD and comparable light yield than EJ-299-33 tested under the same conditions, i.e., figure of merit (FoM) of 1.33 ± 0.03 at 450 keV ee and light yield of 94% relative to EJ-299-33. The 5 wt % PhF-polysiloxane sample had a higher light yield, 144% of EJ-299-33 but lower FoM under the same conditions (FoM of 1.09 ± 0.03). Furthermore, this work highlights the potential of polysiloxanes as a matrix for PSD capable plastic scintillators.

36 MATERIALS SCIENCE↗

Scintillator-based Timepix3 detector for neutron spin-echo techniques using intensity modulation

A scintillator-based Timepix3 (TPX3) detector was developed to resolve the high-frequency modulation of a neutron beam in both spatial and temporal domains, as required for neutron spin-echo experiments. In this system, light from a scintillator is manipulated with an optical lens and is intensified using an image intensifier, making it detectable with the TPX3 chip. Two different scintillators, namely, 6 LiF:ZnS(Ag) and 6 LiI:Eu, were investigated to achieve the high resolution needed for spin-echo modulated small-angle neutron scattering (SEMSANS) and modulation of intensity with zero effort (MIEZE). The methodology for conducting event-mode analysis is described, including the optimization of clustering parameters for both scintillators. The detector with both scintillators was characterized with respect to detection efficiency, spatial resolution, count rate, uniformity, and γ-sensitivity. The 6 LiF:ZnS(Ag) scintillator-based detector achieved a spatial resolution of 200 μm and a count rate capability of 1.1 × 10 5 cps, while the 6 LiI:Eu scintillator-based detector demonstrated a spatial resolution of 250 μm and a count rate capability exceeding 2.9 × 10 5 cps. Furthermore, high-frequency intensity modulations in both spatial and temporal domains were successfully observed, confirming the suitability of this detector for SEMSANS and MIEZE techniques, respectively.

47 OTHER INSTRUMENTATION↗

Activator-doped Hg 2 Br 2 as next generation high performance scintillator for high energy physics research and other scientific and imaging applications

Existing COTS inorganic scintillators all have the characteristic of being very good at certain desirable properties, but not sufficient at other desirable properties for HEP. The demand for suitable scintillators (with regards to both scintillation detector properties and suitable pricing), to be used for modern intensities frontier (Mu2e-II), energy frontier (High luminosity large hadron collider) and future e+e- collider projects (aimed as Higgs bosons factory, such as the International Linear Collider (ILC) and the Future Circular Collider (FCC) are putting even higher challenges on crystal scintillators.In this work, we report the development of a novel high-performance scintillators that can address the issues associated with existing scintillators, the activator doped Hg2Br2. Initial results are very encouraging on the detection of gamma and alpha particles using a solid-state photomultiplier (SSPM). The responses have been stable and repeatable. Hg2Br2 also has many advantages over existing COTS scintillators such as: high density, bright, fast, good energy resolution, no intrinsic radiation, radiation hard and cost-effectiveness. Here, we present here why Hg2Br2 is the next generation scintillator for high energy physics experiments as well as other scientific and imaging applications such as planetary science and medical imaging.

36 MATERIALS SCIENCE↗

Mixed Material Scintillator Systems for Neutron Detection

Scintillators are a fundamental technology that enables radiation detection. Their use has historically enabled the detection of incoming gamma radiation, with recent advances in plastic scintillator development enabling detection and discrimination of neutron and gamma radiation through pulse shape discrimination. However, scintillators have so far consisted of a single material, typically one primary dye and one secondary dye embedded in a plastic matrix. Based on the simulation studies described previously, mixed material scintillator systems with multiple secondary dyes arranged in alternating, periodic micro-sized regions opens the door for scintillators with a wide variety of different capability, such as directional sensing, positional reconstruction, particle identification, and pulse shape discrimination. However, fabrication of a mixed material scintillator system by conventional manufacturing methods is difficult to manufacture and scale, creating a barrier to their wide spread implementation. On the other hand, additive manufacturing additive manufacturing presents itself as the optimal method for fabricating mixed material scintillator systems based on its flexibility, ability to fabricate fine features, and potential for multimaterial fabrication.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DRiFT - Release 1.0.0 Organic Scintillators

DRiFT (a Detector Response Function Toolkit) is LANL-developed software that postprocesses output from the extensively validated radiation transport code, MCNP [1], and generates realistic nuclear instrumentation response. DRiFT is designed to be flexible, enabling users to specify detector type and many experimental settings, as well as accommodating the addition of their own desired features. Although DRiFT development has included scintillator [2], gas [3], and semiconductor features [4], the focus of this release is on organic scintillator and associated capabilities. Organic scintillators are widely used in the areas of nuclear safeguards and nuclear non-proliferation efforts [5, 6]. DRiFT has several diagnostic and detector physics features relevant to detailed scintillator simulations including: tracking source particle information, scintillation light production, the effects of PMT quantum efficiency and gain, and digitizer settings. Users can select responses from many scintillator and PMT types supported natively by DRiFT, or add their own by following the instructions in this document. We acknowledge that DRiFT is under active development, bug reports and general questions and comments should be directed to Madison Andrews, madison@lanl.gov. This manual is divided into four parts: I) An overview of DRiFT, including how to obtain and install the executable, II) A description of the detector physics related to scintillators available, III) a description of more general DRiFT features the user may find useful, and IV) a description of the test suite and examples made available with the code release.

61 RADIATION PROTECTION AND DOSIMETRY↗

DRiFT - Release 1.1.1: Organic Scintillators

DRiFT (a Detector Response Function Toolkit) is LANL-developed software that postprocesses output from the extensively validated radiation transport code, MCNP, and generates realistic nuclear instrumentation response. DRiFT is designed to be flexible, enabling users to specify detector type and many experimental settings, as well as accommodating the addition of their own desired features. Although DRiFT development has included scintillator, gas, and semiconductor features, the focus of this release is on organic scintillator and associated capabilities. Organic scintillators are widely used in the areas of nuclear safeguards and nuclear non-proliferation efforts. DRiFT has several diagnostic and detector physics features relevant to detailed scintillator simulations including: tracking source particle information, scintillation light production, the effects of PMT quantum efficiency and gain, and digitizer settings. Users can select responses from many scintillator and PMT types supported natively by DRiFT, or add their own by following the instructions in this document. We acknowledge that DRiFT is under active development, bug reports and general questions and comments should be directed to Madison Andrews, madison@lanl.gov. This manual is divided into four parts: I) An overview of DRiFT, including how to obtain and install the executable, II) A description of the detector physics related to scintillators available, III) a description of more general DRiFT features the user may find useful, and IV) a description of the test suite and examples made available with the code release.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Solar cycle variation of interplanetary disturbances observed as Doppler scintillation transients

Interplanetary disturbances characterized by plasma that is more turbulence and/or moves faster than the background solar wind are readily defected as transients in Doppler scintillation measurements of the near-Sun solar wind. Systematic analysis of over 23,000 hours of Pioneer Venus Orbiter Doppler measurements obtained inside 0.5 AU during 1979-1987 have made it possible for the first time to investigate the frequency of occurrence of Doppler scintillation transients under solar minimum conditions and to determine its dependence on solar cycle. On the basis of a total of 142 transients, Doppler scintillation transient rates vary from a high of 0.22 in 1979 (one every 4.6 days) to a low of 0.077 transients/d in 1986 (one every 13 days), a decrease by almost a factor of 3 from solar maximum to solar minimum. This solar cycle variation, the strongest yet of any solar wind Doppler scintillation property, is highly correlated with both solar activity characterized by sunspot number and the coronal mass ejection rates deduced from Solswind and Solar Maximum Mission (SMM) coronagraph observations. These results indicate that coronal mass ejections and Doppler scintillation transients are closely related not just during solar maximum, as occasional individual comparisons have shown in the past, but throughout the entire solar cycle, and strengthen the notation that the Doppler scintillation and optical transients are different manifestations of the same physical phenomenon. The magnitudes of the transients, as described by the ratio of peak to pretransient scintillation levels (EF for enhancement factor), and their distribution iwth heliocentric distance also vary with solar cycle. While EF tends to diminish with increasing heliocentric distance during high solar activity, it is more evenly distributed during low solar activity. EF is also lower during solar minimum, as 13% of the transients during solar maximum have values exceeding 23, the highest EF observed during solar minimum. These results are consistent with the fact that occasional major fast-moving interplanetary shocks that are observed during solar maximum are very rate during solar minimum.

Woo, Richard↗

Scintillation Breakdowns in Chip Tantalum Capacitors

Scintillations in solid tantalum capacitors are momentarily local breakdowns terminated by a self-healing or conversion to a high-resistive state of the manganese oxide cathode. This conversion effectively caps the defective area of the tantalum pentoxide dielectric and prevents short-circuit failures. Typically, this type of breakdown has no immediate catastrophic consequences and is often considered as nuisance rather than a failure. Scintillation breakdowns likely do not affect failures of parts under surge current conditions, and so-called "proofing" of tantalum chip capacitors, which is a controllable exposure of the part after soldering to voltages slightly higher than the operating voltage to verify that possible scintillations are self-healed, has been shown to improve the quality of the parts. However, no in-depth studies of the effect of scintillations on reliability of tantalum capacitors have been performed so far. KEMET is using scintillation breakdown testing as a tool for assessing process improvements and to compare quality of different manufacturing lots. Nevertheless, the relationship between failures and scintillation breakdowns is not clear, and this test is not considered as suitable for lot acceptance testing. In this work, scintillation breakdowns in different military-graded and commercial tantalum capacitors were characterized and related to the rated voltages and to life test failures. A model for assessment of times to failure, based on distributions of breakdown voltages, and accelerating factors of life testing are discussed.

Teverovsky, Alexander↗

Scintillation Detector for the Measurement of Ultra-Heavy Cosmic Rays on the Super-TIGER Experiment

We discuss the design and construction of the scintillation detectors for the Super-TIGER experiment. Super-TIGER is a large-area (5.4sq m) balloon-borne experiment designed to measure the abundances of cosmic-ray nuclei between Z= 10 and Z=56. It is based on the successful TIGER experiment that flew in Antarctica in 2001 and 2003. Super-TIGER has three layers of scintillation detectors, two Cherenkov detectors and a scintillating fiber hodoscope. The scintillation detector employs four wavelength shifter bars surrounding the edges of the scintillator to collect the light from particles traversing the detector. PMTs are optically coupled at both ends of the bars for light collection. We report on laboratory performance of the scintillation counters using muons. In addition we discuss the design challenges and detector response over this broad charge range including the effect of scintilator saturation.

Link, Jason↗

Gallium oxide semiconductor-based large volume ultrafast radiation hard spectroscopic scintillators

We report on the development of the first-ever inorganic radiation-hard moisture-insensitive large volume spectroscopic semiconductor-based scintillator with less than 2 ns decay time and light yields as high as 8000 ph/MeV. Despite extensive research into scintillator materials, the quest for an ideal scintillator combining ultrafast decay times (akin to BaF 2 and Yb-doped scintillators such as Lu 2 O 3 :Yb), high light yields (exceeding 2000 photons per MeV), spectroscopic capabilities, and exceptional radiation hardness remain unfulfilled. In this study, we demonstrate and report for the first time the viability of large-volume (up to 20 mm thickness) gallium oxide (β-Ga 2 O 3 ) semiconductor-based scintillators for applications requiring these properties. These β-Ga 2 O 3 scintillators were grown using the fast turnaround (~2 days) crucible-free optical float zone (FZ) technique. The high light yield and ultrafast decay time of these high-purity n-type semiconductors with free carrier concentration of 6 × 10 17 cm –3 are attributed to native defects, specifically oxygen vacancies (V O ) and gallium–oxygen vacancy pairs (V Ga –V O ), generated during optimized FZ growth. The ultrafast decay, along with high light yield, enables excellent timing resolution and high count rate detection for applications like time-of-flight positron emission tomography, physics experiments, and nuclear safety. The radiation hardness of these devices has been documented in a separate publication.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Low Level Calibration of Liquid Scintillation Counting

Liquid Scintillation Counting (LSC) is an analytical laboratory method that quantifies the concentrations of alpha and beta emitting isotopes. The LSC method can be utilized for the detection of tritium, both environmentally and at nuclear facilities. Most LSC samples are aqueous-based and prepared as a radioactive sample dissolved or suspended in a high efficiency scintillation cocktail that converts radioactive energy into light pulses. When placed in counting vials, the liquid scintillation cocktail allows for optical coupling in which energy is released from the samples radioactive decay, and transferred to the scintillator. That energy is then absorbed to produce excited electrons that fall back to their ground-state and emit a pulse of light that is detected by the liquid scintillation analyzers photomultiplier tubes. Quench is a signal attenuation due to physical, chemical, or color interferences. To compensate for quench, quench standards of a known concentration are implemented at increasing increments of quench per vial to create a quench curve. Quench standards can be purchased pre-made or customized from the manufacturer, however, there are several issues that arise from purchasing the pre-made quench standards. The main issues with ordering pre-made quench standards is that they use higher count values, between 30,000 and 250,000 disintegrations per minute (dpm) of tritium per vial and only come in glass vials. Using higher counting standards in glass vials makes it hard to see lower concentrations in plastic vials. Additionally, when using higher energy standards the accuracy of the calibration readings tend to be lower. On the other hand, making a set of quench standards in-house allows for the customization of the dpm concentration to roughly 1,500-3,000 and preparation in plastic vials. This allows for lower activity readings that results in closer precision of the samples' true concentration. Technical Objectives: Create a quench curve and calibrate the LSA for tritium. Verify the calibration of the quench curve prior to cross sample runs. Check calibration against Quality Control (QC) reference value. Conclusion: a tritium quench curve calibration was performed using a scintillation cocktail with ultima gold (AB and AB/F), acetone (only with AB), and water (only with AB/F). By performing the tritium quench curve calibration, the counting efficiency was correlated to various levels of quench. Calibration checks with quality control standards were also performed to verify that the calibration was correct. The observed results provided acceptable values that matched the quality control standard reference values with an acceptable uncertainty. The next step will be fine tuning and cross comparison checks with legacy instrumentation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Influence of fluorescent dopants on the vat photopolymerization of acrylate-based plastic scintillators for application in neutron/gamma pulse shape discrimination

Plastic scintillators, a class of solid-state materials used for radiation detection, were additively manufactured with vat photopolymerization. The photopolymer resins consisted of a primary dopant and a secondary dopant dissolved in a bisphenol A ethoxylate diacrylate-based matrix. The absorptive dopants significantly influence important print parameters, for example, secondary dopants decrease the light penetration depth by a factor > 12×. The primary dopant 2,5-diphenyloxazole had minimal impact on the printing process even when loaded at 25 % by mass of the resin. Working curve measurements, which relate energy dose to cure depth, were performed as a function of feature size to further assess the influence of dopants. Photopatterns smaller than 150 µm width had apparent increases in critical energy dose compared to larger photopatterns, while all resins maintained printed features in line gratings with 50 µm of separation. Printed scintillator monoliths were compared to scintillators cast by traditional molding, demonstrating that the layer-by-layer printing process does not decrease scintillation response. In conclusion, a maximum light output of 31 % of a benchmark plastic scintillator (EJ-200) and successful pulse shape discrimination were achieved with 20 % by mass 2,5-diphenyloxazole as the primary dopant and 0.1 % by mass 9,9-dimethyl-2,7-distyrylfluorene as the secondary dopant in printed scintillator samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Performance evaluation of pulse shape discrimination capable organic scintillators for space applications

Scintillators with pulse-shape discrimination (PSD) capability are of great interest to many fields in the scientific community. The ability to discern a gamma ray from a neutron using PSD varies between different types of scintillator materials and dopants. Here a new generation of organic scintillator materials with PSD capability were studied to determine their radiation hardness to neutron and gamma-ray radiation. The PSD capability, average pulse shapes, and light output of four types of organic scintillator were characterized before and after neutron and gamma-ray irradiation. The main goal of this investigation is to study the effects of long-term irradiation that may be experienced in space applications on the light output and particle discriminating capabilities of each material. EJ-270, EJ-276, organic glass, and Stilbene were tested. Damage due to neutron irradiation (displacement damage) was not observed in any of the scintillators up to 2.56 x 10 11 n/cm 2 , except for Stilbene which showed a small (12%) decrease in light output. All scintillators presented some light output reduction after gamma-ray irradiation (total ionizing dose), with reductions of 17% (EJ-276 and OGS), 32% (EJ-270), and 42% (Stilbene) observed immediately after 100 kRad.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗