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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Luminescence and Scintillation in the Niobium Doped Oxyfluoride Rb4Ge5O9F6:Nb

A new niobium-doped inorganic scintillating oxyfluoride, Rb4Ge5O9F6:Nb, was synthesized in single crystal form by high-temperature flux growth. The host structure, Rb4Ge5O9F6, crystallizes in the orthorhombic space group Pbcn with lattice parameters a = 6.98430(10) Å, b = 11.7265(2) Å, and c = 19.2732(3) Å, consisting of germanium oxyfluoride layers made up of Ge3O9 units connected by GeO3F3 octahedra. In its pure form, Rb4Ge5O9F6 shows neither luminescence nor scintillation but when doped with niobium, Rb4Ge5O9F6:Nb exhibits bright blue luminescence and scintillation. The isostructural doped structure, Rb4Ge5O9F6:Nb, crystallizes in the orthorhombic space group Pbcn with lattice parameters a = 6.9960(3) Å, b = 11.7464(6) Å, and c = 19.3341(9) Å. X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements suggest that the niobium is located in an octahedral coordination environment. Optical measurements inform us that the niobium dopant acts as the activator. The synthesis, structure, and optical properties are reported, including radioluminescence (RL) measurements under X-ray irradiation.

Carone, Darren (ORCID:0000000164014098)↗
DOE OSTI2021

Spatially resolved x-ray detection with photonic crystal scintillators

We study the self-collimation phenomenon in photonic crystals (PhC) of wide bandgap materials for ultra-fast and high spatial resolution x-ray detection. We work on various heavy inorganic scintillators: BaF 2 , GaN, ZnO, CsI:Tl, NaI:Tl, LYSO, WO 4 compounds, and plastic scintillators. Conventional scintillator detectors do not rely on a direct detection mechanism; hence, they require intricate design and fabrication processes. We offer a PhC design to observe self-collimation phenomena and overcome the ongoing spatial resolution challenges with these types of materials. We investigate the photonic band diagrams and iso-frequency contours. Fourier transforms based on finite-difference time-domain and frequency domain simulations are done for verifying and analyzing the self-collimation with the selected material. Light extraction efficiency at the PhC–air interface, depending on the truncation distance from the excitation point, is measured. Beam divergence values are calculated at 1 mm propagation distance. The vertical field profiles are obtained to observe the confinement. For the spatial resolution analysis, cross-sectional beam profiles have been examined. Furthermore, Gaussian envelopes are fitted to beam profiles for a consistent data analysis, and full-width-at-half-maximum values are considered. As a result, we theoretically prove and demonstrate the spatially resolved x-ray detection at the sub-micrometer level for a wide range of scintillator materials.

36 MATERIALS SCIENCE↗
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 OSTI2022

Improved light yield and growth of large-volume ultrafast single crystal scintillators Cs 2 ZnCl 4 and Cs 3 ZnCl 5

Due to their reported fast decay times, Cs 2 ZnCl 4 and Cs 3 ZnCl 5 are promising candidates for detection of gamma rays and X-rays in high count rate and fast timing applications. In this work, we show that single crystals with better optical quality than previously demonstrated – and larger in size – can be grown via the vertical Bridgman method. Highly transparent Ø7 mm crystals of undoped Cs 2 ZnCl 4 and Cs 3 ZnCl 5 are grown and measured to have light yields surpassing those previously reported, achieving 1980 ± 100 ph/MeV and 1460 ± 70 ph/MeV at 662 keV – a 55% and 232% improvement, respectively. We observe single-component scintillation decay times for both Cs 2 ZnCl 4 (1.66 ns) and Cs 3 ZnCl 5 (0.82 ns) and radioluminescence emission with maximum intensity at ~290 nm. Scalability of these materials is also evaluated based on growth of Ø22 mm crystals. Minimal cracking is observed, and the fast decay times are maintained at this size. Coincidence time resolution of 3 × 3 × 5 mm 3 and 7 × 7 × 10 mm 3 pixels cut from Ø22 mm Cs 2 ZnCl 4 are measured to be 148 ± 1 ps FWHM and 175 ± 1 ps FWHM, respectively. Here, the improved performance and ability to be fabricated in large sizes now place Cs 2 ZnCl 4 and Cs 3 ZnCl 5 on the map as potential contenders for radiation detection applications where BaF 2 – the most commonly used ultrafast inorganic scintillator – is typically considered.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Accelerated radiation transport modeling techniques for pencil beam computed tomography using gamma rays

Monte Carlo radiation transport modeling studies were performed for a compact, and high-resolution gamma-ray computed tomography system designed for imaging irradiated nuclear fuel. The system comprises a 60 Co source – chosen for its highly penetrating 1173 keV and 1332 keV gamma rays – a pair of high-aspect-ratio pencil beam collimators, and an inorganic scintillator detector. Here two acceleration methods are proposed to rapidly model a transmission type gamma-ray tomography system. The first, a variance reduction technique, is based on performing Monte Carlo simulations with a monodirectionally-biased source, sampled from a characteristic sub-volume of the full source volume. The second acceleration method is based on the deterministic calculations using the Beer–Lambert law and detector response characteristics. Comparison of simulations using acceleration approaches with analog simulations of the fully isotropic, full-volume equivalent, show that the Monte Carlo variance reduction technique gives quantitatively accurate predictions for large collimator aspect ratios while the deterministic calculations are semi-quantitative but converge close to the correct result as the collimator aspect ratio increases. As such, these techniques can be used to reduce the computational cost in generating simulated radiographs and tomographs by several orders of magnitude. Experimental validation efforts are currently underway and will be demonstrated in future work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Reduction of detection limit and quantification uncertainty due to interferent by neural classification with abstention

Many measurements in the physical sciences can be cast as counting experiments, where the number of occurrences of a physical phenomenon informs the prevalence of the phenomenon's source. Often, detection of the physical phenomenon (termed signal) is difficult to distinguish from naturally occurring phenomena (termed background). In this case, the discrimination of signal events from background can be performed using classifiers, and they may range from simple, threshold-based classifiers to sophisticated neural networks. These classifiers are often trained and validated to obtain optimal accuracy, however we show that the optimal accuracy classifier does not generally coincide with a classifier that provides the lowest detection limit, nor the lowest quantification uncertainty. Here, we present a derivation of the detection limit and quantification uncertainty in the classifier-based counting experiment case. We also present a novel abstention mechanism to minimize the detection limit or quantification uncertainty a posteriori. We illustrate the method on two data sets from the physical sciences, discriminating Ar-37 and Ar-39 radioactive decay from non-radioactive events in a gas proportional counter, and discriminating neutrons from gammas in an inorganic scintillator and report results therefrom.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Gamma-ray imaging of Np-237 metal using an organic glass imager

Neutron and gamma-ray imaging systems are deployed within the field of nuclear safeguards for the detection and localization of special nuclear materials and other materials of interest. 237 Np is one of these materials of interest due its presence in spent nuclear fuel and potential for use in nuclear weapons when purified. Here, for the first time, a 6 kg neptunium sphere (98.8 wt% 237 Np) was measured using a dual-particle imager, from the University of Michigan, consisting of organic glass and inorganic scintillators. The novel composition of organic glass scintillator was recently developed at Sandia National Labs and has been used in particle imaging systems due to its time resolution and particle discrimination capabilities. Gamma-ray energy spectra from single and coincident events were extracted and the sequencing of Compton scatter and photoelectric absorption gamma-ray events was used to generate images using simple backprojection. The emissions of interest in this work are the 312 keV and 416 keV gamma rays from 233 Pa, a daughter isotope from the neptunium decay series. The results of this work show that there is close agreement between the true source location in angular space and the converged location from the gamma ray images created using the system. The gamma spectroscopy from single and coincident events also identified the characteristic emission from the daughter isotope and could be used to assist with the identification of 237 Np. Furthermore, successful localization of the source with 5 s of data demonstrates the practical application of the imaging system for imaging and detection of material in weapons-useable quantities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Monte Carlo simulation of the passage of $\gamma$-rays and $\alpha$-particles in CsI

In this work, theoretical and computational methods for simulating the creation of ionization tracks by fast ions in solids were applied to the passage of a-particles in CsI, an inorganic scintillator commonly used for radiation detection. The methods were implemented in a Monte Carlo program to simulate the interaction of $\alpha$-particles, with incident energies of up to 1 MeV, with CsI. The simulations followed the fate of individual electron-hole pairs and thus allowed for a detailed description of the microscopic structure of ionization tracks created by incident radiation. Simulations were also performed with $\gamma$-rays of the same energy to compare and contrast the ionization tracks obtained with both types of particle. Intrinsic properties such as the mean energy per electron-hole pair, Fano factor, maximum theoretical light yield, and spatial distributions of electron-hole pairs were computed for both $\alpha$-particles and $\gamma$-rays. $\alpha$-particles created cylindrical tracks that were initially aligned with the incident direction and with initial radii of a few nanometers, whereas $\gamma$-rays showed significant scattering, resulting in probability distributions with lower intensities and much greater radial extents.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Detector Materials Scoping Study: Research and Development Recommendations

Radiation detection materials have a unique role in many nuclear security missions. The variety of different applications requires the use of different materials whose characteristics are determined by the specific application requirements. While baseline capabilities have been established to use radiation detection in these applications, the potential to greatly advance those capabilities still exists through the development of superior radiation detection materials and/or the development of new materials that enable new technologies to be implemented more effectively. In 2024 the Defense Nuclear Nonproliferation Research and Development (DNN R&D) Near Field Detection Portfolio charged a detector materials scoping study, composed of a group of radiation-detection materials subject matter experts, to produce a community-wide consensus view of the current state of radiation materials research and to set recommendations for expanded investment over a ten-year time frame. This scoping study sought to understand and document the landscape of how radiation detection materials are used, what characteristics drive the selection of various materials, and what developments are needed to drive the state of the art. To respond to this charge, the scoping study created three working groups, each focusing on a different topical area in radiation detection materials research - Semiconductor Materials, Inorganic Scintillators and Organic Scintillators - with the task to identify the current state of the art in materials research and to provide mission-relevant research and development recommendations. Each working group was chaired by two members of the project team with widely recognized expertise in the field. Solicitations were sent out to experts at the DOE national laboratories, industry, academia and federal government agencies to participate in these working groups. The working groups met at regular intervals throughout 2024 and early 2025, each delivering a technical roadmap designed to enable the pursuit of R&D more intensely on high-impact materials challenges and detector solutions that are deemed as the greatest strategic value to DNN R&D and its stakeholders. The roadmap is also intended to help communicate recommended programmatic priorities within DNN R&D and across the nonproliferation and research communities.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Gamma-ray Spectroscopy in Low-Power Nuclear Research Reactors

Gamma-ray spectroscopy is an effective technique for radioactive material characterization, routine inventory verification, nuclear safeguards, health physics, and source search scenarios. Gamma-ray spectrometers typically cannot be operated in the immediate vicinity of nuclear reactors due to their high flux fields and their resulting inability to resolve individual pulses. Low-power reactor facilities offer the possibility to study reactor gamma-ray fields, a domain of experiments hitherto poorly explored. In this work, we present gamma-ray spectroscopy experiments performed with various detectors in two reactors: The EPFL zero-power research reactor CROCUS, and the neutron beam facility at the Ohio State University Research Reactor (OSURR). We employed inorganic scintillators (CeBr3), organic scintillators (trans-stilbene and organic glass), and high-purity germanium semiconductors (HPGe) to cover a range of typical—and new—instruments used in gamma-ray spectroscopy. The aim of this study is to provide a guideline for reactor users regarding detector performance, observed responses, and therefore available information in the reactor photon fields up to 2 MeV. The results indicate several future prospects, such as the online (at criticality) monitoring of fission products (like Xe, I, and La), dual-particle sensitive experiments, and code validation opportunities.

Pakari, Oskari V. (ORCID:0000000337048190)↗
NASA NTRS2006

Temperature Effects in the ATIC BGO Calorimeter

The Advanced Thin Ionization Calorimeter (ATIC) Balloon Experiment contains a segmented calorimeter composed of 320 individual BGO crystals (18 radiation lengths deep) to determine the particle energy. Like all inorganic scintillation crystals the light output of BGO depends not only on the energy deposited by particles but also on the temperature of the crystal. ATIC had successful flights in 2000/2001 and 2002/2003 from McMurdo, Antarctica. The temperature of balloon instruments varies during their flights at altitude due to sun angle variations and differences in albedo from the ground and is monitored and recorded. In order to determine the temperature sensitivity of the ATIC calorimeter it was temperature cycled in the thermal vacuum chamber at the CSBF in Palestine, TX. The temperature dependence is derived from the pulse height response to cosmic ray muons at various temperatures.

Isbert, J.↗
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 OSTI2021

Fabrication of Low-Cost Large-Volume Ceramic A 2 HfX 6 (A= Cs or Tl, X = Cl, Br, or I) Scintillators for Gamma Ray Detection (SBIR Phase I Final Technical Report)

Scintillator crystals play an important role in the radiation detection field. Widespread use of scintillators as gamma-ray detectors is largely generated by their extensive availability and tunable properties, such high light output, high stopping power (Z eff ), fast decay time, and good proportionality. Additionally, the cost for manufacturing a scintillation detector like NaI:Tl is usually considerably lower than the cost for manufacturing a semiconductor detector like CdZnTe. Because there is no such thing as an ideal scintillation material, an application requiring certain detection characteristics may incorporate a scintillator tailored to its specific properties. The vast variety of applications and requirements necessitates more research into new scintillation materials and/or better methods of producing existing materials.The goal of this project was to grow low cost and environmentally stable inorganic transparent ceramic scintillators with excellent gamma ray resolution, excellent energy proportionality, excellent detection efficiency due to high density (>5 g/cm 3 ) and very high Z eff (55-80), and good light yields (>40,000 ph/MeV). In Phase I Xtallized Intelligence, Inc. (XI, Inc) developed a novel ceramic fabrication technique to produce low cost and environmentally stable highly efficient inorganic transparent ceramic scintillators of various dimensions. XI, Inc., collaborating with Fisk University (Fisk), investigated the scintillation properties of these new ceramic scintillators and compared them to in their single crystal counterparts. The results of this Phase I project show that successful production of high-quality inorganic halide ceramic scintillators Cs 2 HfCl 6 (CHC) and Tl 2 HfCl 6 (THC). Both ceramic CHC and THC scintillators have achieved good performance close to the performance of their single crystal counterparts. Fabricating these inorganic ceramic scintillators mitigate many issues encountered during conventional bulk crystal growth by melt methods. Additional benefits of the ceramic fabrication technique include high production yield, low production cost, fast production time, and no material waste Inorganic transparent ceramic scintillators produced in this project will enhance cost effectiveness at the instrument level based on low projected cost of the proposed compounds, as much smaller crystal sizes would be required to achieve similar efficiency as current radioisotope identification devices (RIID’s) used in homeland security applications as well as spectrometers in high energy physics applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

High-Performance/-Precision/-Z(HPPZ) Scintillator Grids via Advanced Electrochemistry. Phase I – Project # 20210572MFR- Mid year review [Slides]

Scintillation grids with improved imaging resolution in time and space, are required for future mission needs at various facilities (pRad user station, LANSCE, DARHT, Scorpius etc). Current technologies use inorganic crystal scintillators, which are positioned within a high-Z scintillator septa. Dense and high-Z materials are optimal for gamma-ray detection making them promising candidates for development of high -performance/-precision/-Z (HPPZ) scintillator grids. The current resolution of standard chemical etching and fabrication processes of high-Z materials is very low, leading to undesired undercutting and ultimately reducing crystal performance efficiency. Goals are to: Perform initial feasibility studies with the aim of producing complex parts for applications with difficult-to-process high-Z material; Use of pulse and pulse-reverse electrochemical methods on additive approaches to produce high-precision Au and Re scintillator grids at a small scale; and, Follow up in Phase II with the delivery of a large-scale scintillator grid of the best material candidate with unprecedented properties for LANL needs determined in Phase I.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Crystal Growth and Characterization of Europium-Doped Rubidium Calcium Bromide Scintillators

National security strategies like gamma spectroscopy and high-energy X-ray radiography are limited, in part, by the scintillator used, prompting research into novel materials with improved properties. In this paper, Eu 2+ activated rubidium calcium bromide scintillators were grown via the vertical Bridgman method with a range of dopant concentrations. Light yield, energy resolution, and the afterglow of Rb 4 CaBr 6 :Eu and RbCaBr 3 :Eu improved with increasing Eu 2+ concentration, and scintillation decay time increased. The highest light yields of Rb 4 CaBr 6 :Eu and RbCaBr 3 :Eu were 71000 and 45000 ph/MeV, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Scintillating glass for precision calorimetry in nuclear physics

High-performance scintillator materials are needed for particle identification and measurements of energy and momentum of electromagnetic particles in modern nuclear physics experiments. As an example, the US Electron-Ion Collider, a unique collider with diverse physics topics, requires electromagnetic calorimetry enabling high-quality electron identification and detection in the momentum range of 0.3 to tens of GeV. The highest resolution in electromagnetic calorimeters can be provided by homogeneous materials, e.g., lead tungstate crystals. Inorganic glass scintillators have been investigated as an attractive and cost-effective alternative to crystals, that is also easier and faster to manufacture in mass production. In this paper, we discuss progress in the fabrication and characterization of recent scintillating glass samples on both test bench and beam tests. Further, the results are well-reproduced by simulation and are discussed in the context of the Electron-Ion Collider experimental requirements and bench-marked against lead tungstate crystals.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

TlSr 2 I 5 :Eu 2+ - A new high density scintillator for gamma-ray detection

In this paper we report on the scintillation properties of TlSr 2 I 5 doped with Eu 2+ , a novel thallium-containing high-resolution scintillator for gamma-ray spectroscopy. Here, small diameter, good quality crystals of TlSr 2 I 5 :Eu (TSI) with different Eu 2+ concentrations were grown by the vertical Bridgman method. X-ray diffraction measurements show that single crystals of TSI belong to the monoclinic system with space group P2 1 /c. TlSr 2 I 5 has a density of 5.32 g/cm 3 and effective Z of 60. The X-ray excited emission of Eu 2+ doped TlSr 2 I 5 features a broad emission band peaking between 460–470 nm. The light yield of TlSr 2 I 5 crystal doped with 1% Eu 2+ is measured to be ~72,000 ph/MeV with an energy resolution of 2.8% at 662 keV. The scintillation decay time which is characteristic of Eu 2+ shows two components, with 90% of the light in a ~500 ns component and the rest in a longer component of ~3 μs.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗