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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Advanced inorganic halide ceramic scintillators

Research in ceramic scintillators has steadily progressed alongside the research in bulk single crystal scintillator growth. As interest in faster scintillation material production with lower cost increases, more research on scintillating ceramics is needed. Research targeting optimization of optically transparent ceramics that can rival bulk-grown crystals grown may lower cost, increase yield, increase volume, and improve energy resolution in applications and systems currently using sodium iodide and alike. Ceramic scintillators that are dense (>5 g/cm 3 ), have high effective Z (>60), are bright (>40,000 photons/MeV), and are not sensitive to moisture as well as those that can be handled without protection are desired. Ultra-fast ceramic materials are also of interest. This paper presents an equipment design and technique to produce inorganic halide ceramic scintillators Cs 2 HfCl 6 (CHC) and Tl 2 HfCl 6 (THC). Improvements and optimization of CHC and THC ceramic scintillator fabrication are gauged by monitoring the energy resolution and peak position of 137 Cs full energy peak at 662 keV. With a 1-inch diameter CHC ceramic scintillator, energy resolution of 5.4% (FWHM) and light yield of 20,700 ph/MeV are achieved, while with a 16-mm diameter THC ceramic scintillator, energy resolution of 5.1% (FWHM) and light yield of 27,800 ph/MeV are achieved. Decay times of 0.6 μs (21%) and 3.0 μs (79%) are measured for CHC and 0.3 μs (13%) and 1.0 μs (87%) for THC. Here, both ceramic CHC and THC scintillators have similarly good proportionality data when compared to their single crystal counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Beta Radiation Hardness of GYGAG(Ce) Transparent Ceramic Scintillators

GYGAG(Ce) transparent ceramic garnet scintillators were irradiated with electrons from 0.5 to 2 MeV with fluences from 10 16 e – /cm 2 to 10 19 e – /cm 2 , corresponding to doses from 0.3 to 310 Gigarad. Absorption spectra were measured before and after irradiations. Light yields from alpha, beta, and gamma excitations were measured before and after irradiation and compared to preirradiation values to gain a deeper understanding of how electron irradiations can affect light yield, as well as defects generated in both the surface and bulk. Within experimental error, no degradation in light yield was observed for the electron-irradiated samples, as measured via beta or gamma excitation, with minimal degradation observed via alpha excitation. A small increase in optical absorption near the wavelength of emission was observed following the largest dose irradiation. These results suggest that GYGAG(Ce) is radiation hard to electron irradiation up to 10 19 e – /cm 2 and doses up to 310 Gigarad. Furthermore, this robustness to irradiation indicates that transparent ceramic garnets may prove useful for applications such as scintillation-based nuclear batteries by allowing for higher energy beta emitters, increased power densities, and enabling long service lifetimes.

36 MATERIALS SCIENCE↗
DOE OSTI2026

HIGHER EFFICIENCY FISSION COUNTER FOR NEUTRON DETECTION

Fission chambers containing 235U have been used for detection of neutrons for many decades. In these chambers 235U is electroplated on a metal which is one plate of an ionization chamber. Since the range of fission products from induced fission in the chamber is extremely short, these deposits from electroplating are so thin that the amount of 235U results in low neutron detection efficiency and the chamber needs high internal 235U surface area to increase efficiency. A typical ~8 in. long, ~2 in. diameter fission counter only contains < 2 g of 235U total, resulting in very low detection efficiency per incident neutron impinging on the outer surface of the detector. However, because of their large electronic pulses from fission products compared to gamma rays it is very easy to discriminate against gamma rays impinging on the detector. These types of chambers are produced commercially and are used worldwide in nuclear research and nuclear power reactors. ORNL has made a higher efficiency fission ionization chamber by using many thin concentric annuli to increase the area. A higher efficiency fission counter would be useful and can be made by incorporating 235U into a glass or ceramic scintillator. For nearly 100 years the green color in antique glass was produced by incorporation of depleted uranium (up to 20 wt. %) into a glass. The concept for this scintillation-optical-based fission detector is to dope a scintillator (either ceramic or glass) with 235U. Glass scintillators are commercially available doped with as much as 8 wt. % 6Li for neutron detection. In the 235U doped scintillator the fission product pulses would be double the size of those in an ion chamber since all fission products produce light in the scintillator whereas in the ionization chamber half do not go into the ionizing gas volume. These higher efficiency fission chambers would be very useful for a wide variety of research, nuclear research, and nuclear power reactor applications. Because of their smaller size and weight, they should be useful for space application such as monitoring of space nuclear power reactors. This report reviews existing fission chamber technology and suggests the development of these small high-efficiency fission chambers. Other fission isotopes could be used for other research applications.

Mihalczo, John [ORNL] (ORCID:0000000254292681)↗
DOE OSTI2022

Novel Ultrafast Lu2O3:Yb Ceramics for Future HEP Applications

Inorganic scintillators activated by charge transfer luminescence Yb3+ are considered promising ultrafast material to break the ps timing barrier for future high energy physics applications. Inorganic scintillators in ceramic form are potentially more cost-effective than crystals because of their lower fabrication temperature and no need for aftergrowth mechanical processing. This paper reports an investigation on Lu2O3:Yb and Lu2xY2(1−x)O3:Yb scintillating ceramic samples fabricated by Radiation Monitoring Devices Inc. All samples show X-ray excited luminescence peaked at 370 nm. Ultrafast decay time of 1.1 ns was observed by using a microchannel plate-photomultiplier tube-based test bench at Caltech. Considering its intrinsic high density (9.4 g/cm3), Lu2O3:Yb ceramics are promising for future time of fight application for high energy physics experiments.

47 OTHER INSTRUMENTATION↗
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

Thermal Processing Conditions for the Synthesis of Near Theoretical Density Li 5 La 3 Ta 2 O 12 Ceramics for Ceramic Dual-Mode Detectors

A family of Li-containing garnet compounds, extensively investigated for Li-ion solid electrolyte applications, show great potential to be developed into transparent ceramic dual-mode scintillators. In particular, Li 5 La 3 Ta 2 O 12 (LLTaO) shows promise as an efficient dual-mode scintillator due to its high Li content, high density, non-hygroscopicity, and high effective-Z. Often the synthesis of LLTaO ceramics involves solid state processing techniques starting with oxide and carbonate powders, calcining, sintering for the removal of residual porosity, and post-processing. This study focuses on two objectives: (1) establishing thermal processing boundary conditions for a flexible alkoxide-based sol-gel method for synthesizing fine-grained powders; and (2), consolidating powders via hot-pressing to form high-density ceramics. In this study, near single-phase ceramics were achieved by hot-pressing sol-gel powders with varying amounts of excess Li. Rietveld refinements were used to analyze X-ray diffraction data and provide a quantitative evaluation of the phases present in the hot pressed ceramics. Some of the diffraction data showed large low angle peak asymmetry, suggesting the presence of two cubic Li 5 La 3 Ta 2 O 12 garnet phases with different lattice parameters. Depending on the synthesis and processing conditions, the refinement revealed ~ 90 wt% concentration of a phase with a ≈ 12.8 Å and ~ 10 wt% concentration of a phase with a ≈ 12.9 Å, indicating a remaining excess of Li in the hot pressed ceramics in the large lattice parameter phase. These synthesis experiments allowed for the determination of a baseline for Li loss during hot-pressing. X-ray excited radioluminescence and photoluminescence excitation and emission spectra were obtained from the hot pressed ceramics. In conclusion, the measured emission spectra featured broad tantalate emission and line emissions likely from a rare-earth impurity.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Hadron-Induced Radiation Damage in Fast Heavy Inorganic Scintillators

Fast and heavy inorganic scintillators with suitable radiation tolerance are required to face the challenges presented at future hadron colliders of high energy and intensity. Up to 5 GGy and 5 × 1018 neq/cm2 of one-MeV-equivalent neutron fluence is expected by the forward calorimeter at the Future Hadron Circular Collider. This paper reports the results of an investigation of proton- and neutron-induced radiation damage in various fast and heavy inorganic scintillators, such as LYSO:Ce crystals, LuAG:Ce ceramics, and BaF2 crystals. The experiments were carried out at the Blue Room with 800 MeV proton fluence up to 3.0 × 1015 p/cm2 and at the East Port with one MeV equivalent neutron fluence up to 9.2 × 1015 neq/cm2, respectively, at the Los Alamos Neutron Science Center. Experiments were also carried out at the CERN PS-IRRAD proton facility with 24 GeV proton fluence up to 8.2 × 1015 p/cm2. Research and development will continue to develop LuAG:Ce ceramics and BaF2:Y crystals with improved optical quality, F/T ratio, and radiation hardness.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Hot-pressed 6 LiInSe 2 for use as a ceramic radiation detector

Lithium based chalcogenides have many uses in the nuclear science field. 6 LiInSe 2 (or LISe) has been researched extensively because of its ability to operate in both scintillator and semiconductor modes. Here, this makes it useful in applications including nuclear material detection for national security, space applications, and medical imaging. In some applications growth and fabrication costs are of concern, as it takes upwards of 40 days to synthesize a charge, grow a crystal and fabricate a detector. Ceramics are a solution for this long route of preparation. This research shows that using a 6 LiInSe 2 ceramic instead of a single crystal significantly decreases the time required to make a detector. In the present work, ceramic wafers can be formed using a mechanical press equipped with a heating attachment. The resulting ceramic wafer performs very similar to a slow-growth single crystal when used in the scintillator mode.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Proton damage in (Y,Lu,Gd) 3 (Al,Ga) 5 O 12 :Ce mixed garnet scintillators

Scintillators are vital components for nuclear instrumentation and its applications, including plasma diagnostics and imaging. As yields in controlled fusion experiments increase, the radiation tolerance of scintillator candidates for use in instrumentation is of particular importance. High radiation exposure can damage scintillating materials and alter the optical properties. The effects of radiation damage in Ce-doped mixed garnet ceramics over the compositional range (Y,Gd,Lu) 3 (Al,Ga) 5 O 12 are investigated using optical techniques. The samples were exposed to 200 keV protons to an accumulated fluence of 10 16 protons per square centimeter, then characterized using diffuse reflectance spectroscopy (DRS). DRS with visible light can assess the radiation tolerance of opaque poly-crystalline samples, which can be easily sintered from powders and thus offer distinct advantages in characterization compared to single crystals. Qualitative trends in induced absorption are presented as a function of composition, and the ideal cerium dopant concentration for Y 2 LuAl 5 O 12 is determined to be 0.60–0.75 mol.%.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Serrated flow in $\mathrm{NaI:Tl}$ scintillator crystals

We report the serrated-flow behavior is an important phenomenon that unveils material-deformation mechanisms, as reported for various kinds of materials. NaI doped with Tl (NaI:Tl) is unique among scintillation materials in that the structure contains glide planes that are linked to serration behavior. In the present work, single crystals of NaI:Tl were subjected to room-temperature compression experiments at different strain rates. The serrated flow was observed, and complexity and multifractal analyses were performed to analyze the serration behavior. The findings revealed that the strain rate had a pronounced effect on the complexity and multifractality of the serrated flow, similar to what has been found in other alloy systems. The results also indicate that there may be a strong link between the complexity of the serrated flow behavior and the heterogeneity of the underlying dynamics. It is expected that the present work could be a step toward a better understanding of the deformation behavior and forgeability of NaI:Tl single crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ceramic radiation detector device and method

A ceramic lithium indium diselenide or like radiation detector device formed as a pressed material that exhibits scintillation properties substantially identical to a corresponding single crystal growth radiation detector device, exhibiting the intrinsic property of the chemical compound, with an acceptable decrease in light output, but at a markedly lower cost due to the time savings associated with pressing versus single crystal growth.

Preston, Jeffrey R.↗