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DOE OSTI2020

Compound pulse characteristics of a heterogeneous composite scintillator in a gamma-ray field

An important aspect of radiation detection in scintillators is the time dependence of emitted fluorescence, which results in characteristic measured pulse shape. In some materials, a relatively strong dependence of the scintillation pulse shape on stopping power exists, which can provide reliable identification of the incident particle. An alternative method to realize particle identification is by combining materials with different fluorescence lifetimes into heterogeneous structures. Such composite scintillators derive their properties from both the constituent material characteristics and the geometry of the composite structure. In composite scintillators with a high degree of heterogeneous loading, a superposition of fluorescence contributions originating in multiple materials, which is observed as single waveform with an intermediate pulse shape, may affect its ability to reject rays. We measure the time dependence of light output from a scintillator composed of 6 Li-containing glass shards and scintillating polyvinyl toluene and identify events that exhibit such compound behavior when exposed to rays and fast neutrons. We develop a modeling and simulation framework that reproduces the pulse shapes in heterogeneous scintillators and use it study the effect that the weight percentage of 6 Li glass has on rejection. The modeling framework is applied to the experimentally studied scintillator, finding a good agreement. Here, the developed modeling and simulation approach will help optimize the design of heterogeneous scintillators to meet the desired trade-o between neutron capture efficiency and -ray rejection.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Enhancing the Cherenkov over scintillation ratio using dichroic filters in BGO and TlCl for TOF-PET

Abstract The Cherenkov emission in inorganic crystal scintillators has been shown to dramatically improve time resolution for time-of-flight positron emission tomography (TOF-PET) for in slow scintillators with a high refractive index such as bismuth germanium oxide (BGO). This is due to the faster nature of the Cherenkov emission (tens of picoseconds) with respect to scintillation (nanosecond). However, the presence of slower scintillation light and the inability of existing detectors to distinguish between Cherenkov and scintillation make it difficult for BGO to achieve a good CTR for all the detected coincidence events. In this paper, we exploit the difference between the Cherenkov and scintillation emission spectra and use dichroic filters to enhance the Cherenkov over scintillation ratio. Dichroic filters transmit or reflect photons based on their wavelength, with a photon attenuation lower than 10%. We investigate several shortpass and longpass dichroic filters in a single-photon configuration with BGO and find the optimal filter that maximizes the Cherenkov over scintillation ratio. We demonstrate that we can enhance the ratio of Cherenkov to scintillation photons by a factor of 2.17 ± 0.38 by employing a shortpass dichroic filter with a cut-off wavelength of 450 nm for BGO, and by a factor of 2.87 ± 0.40 using a longpass dichroic filter with a cut-on wavelength of 550 nm for iodine/beryllium-doped thallium chloride.

Science & Technology - Other Topics↗

DOE OSTI2024

Scintillation of colloidal nanocrystals

Scintillators are materials that convert ionizing radiation in the form of particles or photons into low-energy photons in the ultraviolet to near-infrared spectral range. Here, this work reviews efforts to use colloidal nanocrystals as scintillator materials. To date, research on colloidal nanocrystals as scintillators has focused on doped phosphor systems, quantum dots and related structures, and perovskite-based nanocrystals. Among various material classes and forms, colloidal semiconductor nanocrystals stand out thanks to their appealing fluorescence properties, yet understanding of their radioluminescence and cathodoluminescence is incomplete. This review discusses fundamental limits and material design challenges toward achieving high brightness, fast speed, and durable scintillator performance with nanocrystal scintillators. First, this review describes the basic principles and efficiency limitations of scintillation, particularly the large influence of multiple exciton generation in many nanocrystal species, as well as performance metrics. Second, methods for measurement are described. Third, we review the results of the main classes of nanocrystal scintillators, including quantum dots and related particles, perovskites, and doped-phosphor particles. Fourth, scintillation imaging is discussed in terms of the relevant performance metrics and results obtained using nanocrystal materials. Finally, we note the strengths and weaknesses of nanocrystal scintillators and discuss potential areas of further development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Scintillation of liquid nitrogen

Liquid nitrogen is commonly used in cryogenic applications and is a promising medium for the direct immersion cooling of sensors used for nuclear and particle physics experiments. The scintillation properties of gaseous nitrogen are well-documented, but little is known about the scintillation of liquid nitrogen. If present, scintillation light from interactions of ambient radioactivity could produce backgrounds for rare event searches such as the direct detection of dark matter. Using a coincidence-tagged alpha decay, we demonstrate that liquid nitrogen exhibits measurable, albeit very faint, scintillation. Assuming the same scintillation wavelengths as gaseous nitrogen, we estimate a relative scintillation yield of $Y_{\liquidn}/Y^{\STP}_{\gasn} =$ \num[uncertainty-descriptors={stat,sys}]{0.0142(0.0005)(0.0030)} with respect to gaseous nitrogen at standard temperature and pressure. Considering the average scintillation yield from alpha decays in gaseous nitrogen, this implies a scintillation yield for alpha decays in liquid nitrogen of $Y_{\liquidn} = \qty[]{2.39(0.56)}{photons~per~MeV}$. To our knowledge this is the first measurement of scintillation in liquid nitrogen.

Pagani, Luca (ORCID:0000000234692581)↗

NASA NTRS1998

Studies of Avalanche Photodiodes (APDS) as Readout Devices for Scintillating Fibers for High Energy Gamma-Ray Astronomy Telescopes

New gamma ray and charged particle telescope designs based on scintillating fiber arrays could provide low cost, high resolution, lightweight, very large area and multi radiation length instrumentation for planned NASA space exploration. The scintillating fibers low visible light output requires readout sensors with single photon detection sensitivity and low noise. The sensitivity of silicon Avalanche Photodiodes (APDS) matches well the spectral output of the scintillating fibers. Moreover, APDs have demonstrated single photon capability. The global aim of our work is to make available to NASA a novel optical detector concept to be used as scintillating fiber readouts and meeting the requirements of the new generations of space-borne gamma ray telescopes. We proposed to evaluate the feasibility of using RMD's small area APDs ((mu)APD) as scintillating fiber readouts and to study possible alternative (mu)APD array configurations for space borne readout scintillating fiber systems, requiring several hundred thousand to one million channels. The evaluation has been conducted in accordance with the task description and technical specifications detailed in the NASA solicitation "Studies of Avalanche Photodiodes (APD as readout devices for scintillating fibers for High Energy Gamma-Ray Astronomy Telescopes" (#8-W-7-ES-13672NAIS) posted on October 23, 1997. The feasibility study we propose builds on recent developments of silicon APD arrays and light concentrators advances at RMD, Inc. and on more than 5 years of expertise in scintillating fiber detectors. In a previous program we carried out the initial research to develop a high resolution, small pixel, solid-state, silicon APD array which exhibited very high sensitivity in the UV-VIS spectrum. This (mu)APD array is operated in Geiger mode and results in high gain (greater than 10(exp 8)), extremely low noise, single photon detection capability, low quiescent power (less than 10 (mu)W/pixel for 30 micrometers sensitive area diameter) and output in the 1-5 volt range. If successful, this feasibility study will make possible the development of a scintillating fiber detector with unsurpassed sensitivity, extremely low power usage, a crucial factor of merit for space based sensors and telescopes.

Vasile, Stefan↗

DOE OSTI2023

Optical Relays for Imaging Scintillators

Cygnus is a dual beam high-energy radiographic x-ray source. Ten years ago, three large zoom lenses were assembled to collect images from 200 mm x 200 mm square scintillators. The zoom capability allows zooming down to a 60 mm x 60 mm picture from the scintillator. Current radiographic imaging needs now require larger 270 mm x 270 mm square scintillators and the capability to use both 92 mm x 92 mm and 62 mm x 62 mm CCD cameras, and a new lens design to meet these needs. This zoom lens incorporates 11 elements and is designed to be telecentric. It images a scintillator emitting light peaking at 435 nm, so special glass types are required for the lens elements. Much larger elliptical pellicles are needed to deflect the scintillator light out of the x-ray path into the lens. The optical axis of the imaging system must be colinear with the x-ray axis. Two scintillators are positioned in each of two Cygnus x-ray axes, for a total of four scintillators and four lens systems. An optional configuration will be shown, enabling two lens systems imaging opposite sides of a single scintillator, for a total of four lenses and two scintillators. Although this configuration has advantages, it suffers from crosstalk. Care must be taken to analyze the anti-reflection coatings applied to all the elements in the imaging chain, including the CCD array and

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2020

Advances in High Resolution Ultrafast Scintillators for Fast timing Applications

Scintillation detectors exhibiting high spatial resolution and fast timing capabilities are of vital importance for synchrotron sources. These detectors may be exposed to a variety of X-ray energies (up to 140 keV) and used in high frame rate applications. Here, we describe the advances in the development of thin-film LuI3:Ce scintillators for higher energy X-ray imaging, with fast timing and high spatial resolution. When grown in a single crystalline form, these scintillators are bright, producing 115 000 photons/MeV. However, to achieve high spatial resolution, these scintillators are grown in thin-film form with a microcolumnar structure, controllable to column diameters of <1-30 mu m. Thus, a much thicker scintillator layer (10 mu m-3 mm or higher) may be grown, providing superior X-ray absorption while achieving high resolutions of 50 mu m or better, at the cost of reduced light yield. To study the timing characteristics of the scintillator, time-resolved X-ray excited optical luminescence (TR-XEOL) was performed on two different sets of three samples of LuI3 at the 1-BM beamline of the Advanced Photon Source at Argonne National Laboratory. Besides, we report timing measurements obtained using a photomultiplier tube (PMT) and oscilloscope at Radiation Monitoring Devices (RMD) Inc. Using the TR-XEOL, we determined the decay constants of LuI3 as a function of Ce doping, recording a fast decay component as low as 3.6 ns (39%), one of the fastest values recorded in inorganic scintillators. This fast decay opens up numerous novel applications, where ultrahigh frame rates are important using synchrotron X-rays. This article will discuss fabrication, characterization, and potential applications for this novel scintillator.

fast timing↗

DOE OSTI2023

Melt Blending: A Tool to Simplify Plastic Scintillator Synthesis

Plastic scintillators are widely used as radiation detection media in homeland security and nuclear physics applications. Their attributes include low cost, scalability to large detector volumes, and additive compounding to enable additional material and detection features, such as pulse shape discrimination (PSD), gamma-ray spectroscopy, aging resistance, and coincidence timing. However, traditional chemically cured plastic scintillators (CCS) require long reaction times, and hazardous wet chemical procedures performed by specially trained personnel, and can leave residual monomer, resulting in deleterious optical and material properties. Here, we synthesize melt blended scintillators (MBSs) in 2.5 days using easily accessible solid-state compounding of commercially-available poly(styrene) with 30–60 wt% fluorene-based compound “P2” to create monolithic detectors with < 100 ppm residual monomer, in several form factors. Further, the best scintillation performance was recorded for 60 wt% P2 in Styron 665, including gamma-ray light yield 139% of EJ- 200 commercial scintillator and PSD figure of merit (FOM) value of 2.65 at 478 keVee, approaching P2 organic glass scintillator (OGS). The capability of MBS to generate fog-resistant scintillators and poly(methyl methacrylate) (PMMA)-based scintillators for use in challenging environments is also demonstrated.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2020

Measuring Thickness-Dependent Relative Light Yield and Detection Efficiency of Scintillator Screens

Digital camera-based neutron imaging systems consisting of a neutron scintillator screen optically coupled to a digital camera are the most common digital neutron imaging system used in the neutron imaging community and are available at any state-of-the-art imaging facility world-wide. Neutron scintillator screens are the integral component of these imaging system that directly interacts with the neutron beam and dictates the neutron capture efficiency and image quality limitations of the imaging system. This work describes a novel approach for testing neutron scintillators that provides a simple and efficient way to measure relative light yield and detection efficiency over a range of scintillator thicknesses using a single scintillator screen and only a few radiographs. Additionally, two methods for correlating the screen thickness to the measured data were implemented and compared. An example 6LiF:ZnS scintillator screen with nominal thicknesses ranging from 0–300 μm was used to demonstrate this approach. The multi-thickness screen and image and data processing methods are not exclusive to neutron scintillator screens but could be applied to X-ray imaging as well. This approach has the potential to benefit the entire radiographic imaging community by offering an efficient path forward for manufacturers to develop higher-performance scintillators and for imaging facilities and service providers to determine the optimal screen parameters for their particular beam and imaging system.

42 ENGINEERING↗

DOE OSTI2021

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↗

DOE OSTI2022

Pulse-shape discrimination in water-based scintillators

This work describes a class of liquid scintillators that contain mostly water (>50 wt% of the entire composition) and can discriminate between interactions induced by neutrons and gamma rays. Here, by balancing the interface interactions between the components of the formulation, these scintillators form emulsions that can be thermodynamically stable. This approach, which considers a quantity known as the hydrophilic–lipophilic difference, requires consideration of the salinity and temperature as well as characterization of the surfactants and oil phase. Emulsions comprised of water and various oils were characterized first. Then, the effect of scintillating dyes in the oil phase was considered, followed by the construction of partial phase diagrams of the emulsions. For transparent oil-in-water emulsions with a single phase, the scintillation light yield and metrics related to pulse-shape discrimination were measured. The best performing scintillators contained 33 wt% of a scintillating oil phase and exhibited a light yield that was as high as 18% of the light yield of a commercially available liquid scintillator that does not contain water (EJ-309). These water-based liquid scintillators exhibited a figure of merit of neutron/gamma ray discrimination as high as 1.79 at about 1500 keV ee .

36 MATERIALS SCIENCE↗

DOE OSTI2026

Picosecond measurements of plastic scintillator pulse shapes from gamma-ray interactions

An understanding of the pulse shape of organic scintillators can provide insight into scintillation mechanisms and inform the selection of the optimal detector material for a given application. Although the timing properties of organic scintillators have been extensively studied, significant discrepancies persist in reported rise and decay times. New plastic scintillating media have also been developed in recent years for which no literature data exist. The goal of this work is to provide high-precision measurements of the pulse shape of a suite of fast plastic organic scintillators from Eljen Technology—EJ-200, EJ-204, EJ-208, EJ-230, EJ-232, and EJ-232Q (with 0.5% benzophenone)—under excitation from $γ$-ray sources. The contributors to the system temporal resolution were quantified, and the dominant source of uncertainty was identified as the determination of the start time of a scintillation event. A pulse shape model was applied to the reconstructed temporal distributions, and rise and decay times were extracted and compared with manufacturer specifications. This work outlines a measurement approach to obtain the pulse shape of organic scintillators in response to $γ$-rays with temporal resolution on the order of tens of picoseconds, yielding data required for modeling plastic scintillator based detection systems for a range of applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Simultaneous measurement of organic scintillator response to carbon and proton recoils

Organic scintillators are widely used for neutron detection in both basic nuclear physics and applications. While the proton light yield of organic scintillators has been extensively studied, measurements of the light yield from neutron interactions with carbon nuclei are scarce. Demonstrate a new approach for the simultaneous measurement of the proton and carbon light yield of organic scintillators. Provide new carbon light yield data for the EJ-309 liquid and EJ-204 plastic organic scintillators. A 33-MeV 2 H + beam from the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory was impinged upon a 3-mm-thick Be target to produce a high-flux, broad-spectrum neutron beam. The double time-of-flight technique was extended to simultaneously measure the proton and carbon light yields of the organic scintillators, wherein the light output associated with the recoil particle was determined using np and nC elastic scattering kinematics. The proton and carbon light yield relations of the EJ-309 liquid and EJ-204 plastic organic scintillators were measured over a recoil energy range of approximately 0.3 to 1 MeV and 2 to 5 MeV, respectively, for EJ-309, and 0.2 to 0.5 MeV and 1 to 4 MeV, respectively, for EJ-204. Furthermore, these data provide new insight into the ionization quenching effect in organic scintillators and key input for simulation of the response of organic scintillators for both basic science and a broad range of applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Metal Halide Scintillators with Fast and Self‐Absorption‐Free Defect‐Bound Excitonic Radioluminescence for Dynamic X‐Ray Imaging

Abstract Scintillators for radiation detection are of great significance in medical imaging, security, and nondestructive inspection. The current challenge for scintillators is to simultaneously achieve high scintillation light yield, fast radioluminescence, simple film fabrication, large X‐ray attenuation efficiency as well as stable and nontoxic compositions; no previous scintillators fulfill all the above requirements. Here, metal halide Rb 2 AgBr 3 , possessing defect‐bound excitonic radioluminescence, is shown as efficient and fast scintillators. This nontoxic and stable scintillator emits from excitons bound to neutral bromine vacancies, enjoying an efficient and spin‐allowed fast emission with minimized self‐absorption. Rb 2 AgBr 3 thus has a high light yield (25 600 photons MeV −1 ), fast scintillation decay time (5.31 ns), and a record value of light yield versus decay time (4821 photons MeV −1 ns −1 ). The close‐space sublimation method is developed for fast and scalable fabrication of oriented Rb 2 AgBr 3 films. The scintillator film is further integrated with commercial flat‐panel imagers, and the spatial resolution reaches 10.2 line pairs per millimeter at the modulation transfer function of 0.2, doubling the resolution of conventional CsI:Tl flat‐panel detectors. The dynamic X‐ray imaging and its use to real‐time monitoring of bone movement without ghosting effect is also demonstrated.

Zhang, Muyi↗

DOE OSTI2024

Scintillation event imaging with a single photon avalanche diode camera

Position and time measurements of scintillation events encode information about the radiation source. Single photon avalanche diode (SPAD) arrays offer multiple-megapixel spatial resolution and tens of picoseconds temporal resolution for detecting single photons. Current lensless designs for measuring scintillation events use sensors that are lower in spatial resolution. Camera-based designs use sensors that are lower in temporal resolution or readout rate and cannot image individual interactions. Here we propose to image scintillation events in a thick, monolithic scintillator using a high-resolution SPAD camera. We demonstrate that a commercial SPAD camera is able to gather sufficient signal to image individual scintillation events and observe 3D shifts in their spatial distribution. Simulations show that a SPAD camera can localize individual scintillation events in 3D. We report direct imaging of gamma-ray interactions in a scintillator with a SPAD camera. The proposed design may allow to measure complex signatures of individual particles interacting in the scintillator.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Scintillation and cherenkov photon counting detectors with analog silicon photomultipliers for TOF-PET

Objective. Standard signal processing approaches for scintillation detectors in positron emission tomography (PET) derive accurate estimates for 511 keV photon time of interaction and energy imparted to the detection media from aggregate characteristics of electronic pulse shapes. The ultimate realization of a scintillation detector for PET is one that provides a unique timestamp and position for each detected scintillation photon. Detectors with these capabilities enable advanced concepts for three-dimensional (3D) position and time of interaction estimation with methods that exploit the spatiotemporal arrival time kinetics of individual scintillation photons. Approach. In this work, we show that taking into consideration the temporal photon emission density of a scintillator, the channel density of an analog silicon photomultiplier (SiPM) array, and employing fast electronic readout with digital signal processing, a detector that counts and timestamps scintillation photons can be realized. To demonstrate this approach, a prototype detector was constructed, comprising multichannel electronic readout for a bismuth germanate (BGO) scintillator coupled to an SiPM array. Main Results. In proof-of-concept measurements with this detector, we were able to count and provide unique timestamps for 66% of all optical photons, where the remaining 34% (two-or-more-photon pulses) are also independently counted, but each photon bunch shares a common timestamp. We show this detector concept can implement 3D positioning of 511 keV photon interactions and thereby enable corrections for time of interaction estimators. The detector achieved 17.6% energy resolution at 511 keV and 237 ± 10 ps full-width-at-half-maximum coincidence time resolution (CTR) (fast spectral component) versus a reference detector. We outline the methodology, readout, and approach for achieving this detector capability in first-ever, proof-of-concept measurements for scintillation photon counting detector with analog silicon photomultipliers. Significance. The presented detector concept is a promising design for large area, high sensitivity TOF-PET detector modules that can implement advanced event positioning and time of interaction estimators, which could push state-of-the-art performance.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2023

Status of Scintillator Development at Fermilab

Fermilab has had a 20+ year history in producing scintillator and is now one of the largest producers of organic scintillator in the world. Its scintillator has been used in a wide variety of applications including archeology, volcanology, mining exploration, agriculture, national security, as well as more traditional applications in HEP and Astro-particle physics. We will survey these applications. We have a scintillator extrusion facility and recently we have added injection molding capacity. We will discuss ongoing and near-term future projects for these facilities. We discuss ongoing R&D to improve light yield and timing performance of the extruded scintillator and hence reduce cost. We will discuss methods to improve light yield of injection-molded scintillator by refinements in the scintillator chemistry and process. Finally, we will present longer-term future plans for making new scintillating materials tailored for specific applications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS2013

Observations of Global and Regional Ionospheric Irregularities and Scintillation Using GNSS Tracking Networks

The rate of TEC index (ROTI) is a measurement that characterizes ionospheric irregularities. It can be obtained from standard GNSS dual-frequency phase data collected using a geodetic type of GNSS receiver. By processing GPS data from ground-based networks of International GNSS Service and Continuously Operating Reference Station (CORS), ROTI maps have been produced to observe global and regional scintillation activities. A major mid-latitude scintillation event in the contiguous United States is reported here that was captured in ROTI maps produced using CORS GPS data collected during a space weather storm. The analyses conducted in this work and previously by another group indicate that ROTI is a good occurrence indicator of both amplitude and phase scintillations of GPS L-band signals, even though the magnitudes of ROTI, S4, and sigma(sub phi) can be different. For example, our analysis indicates that prominent ROTI and the L1 phase scintillation (sigma(sub phi)) are well correlated temporally in the polar region while L1 amplitude scintillation rarely occurs. The differences are partially attributed to physics processes in different latitude regions, such as high-speed plasma convection in the polar region that can suppress the amplitude scintillation. An analysis of the impact of ionospheric scintillation on precise positioning, which requires use of dual-frequency phase data, is also conducted. The results indicate that significant (more than an order of magnitude) positioning errors can occur under phase scintillation conditions.

ionospheric measurements↗