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Project Outline: • Experimental validation of machine learning based prediction models; • Evaluating double perovskite halides (chlorides, some bromides) – A 2 bb'X 6 :Ce; A = Br + , Cs + ; B = Na + , K + ; B' = RE 3+ ; X = Cl - , Br - ; • Performing single crystal growth and characterization (physical, optical, scintillation properties).
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.
The present invention provides for a composition comprising an inorganic scintillator comprising an optionally lanthanide-doped barium mixed halide, useful for detecting nuclear material.
The present invention provides for a composition comprising an inorganic scintillator comprising an optionally lanthanide-doped cesium barium halide, useful for detecting nuclear material.
Objectives: Provide experimental data to feed back in to models for high-throughput predictions of potential new scintillator materials and identify promising scintillator compounds to pursue further.
Inorganic halides (e.g., inorganic halide scintillators) of the general formula A3B2X9, including inorganic halides comprising thallium monovalent cations and/or combinations of different halides, are described. Radiation detectors including the inorganic halide scintillators and methods of using the detectors to detect high energy radiation are also described. In some cases, the scintillators can include a gadolinium cation, a boron cation, a lithium cation, a chloride ion, or combinations thereof and the scintillator can be used to detect neutrons.
X-ray radiography systems are a key national security technology enabling non-invasive cargo screening. However, the scintillators currently used in these systems have limitations in performance that prompt research for new suitable materials. Here, in this work, crystal growth, physical properties, and optical and scintillation properties of a new halide perovskite scintillator RbSrI 3 were investigated for the first time. The melting point was determined to be 453 °C. Divalent europium and ytterbium were investigated as potential luminescent activators. Light yield and energy resolution of RbSrI 3 :Eu 5 mol% was 78,700 ph/MeV and 2.8 % at 662 keV, and that of RbSrI 3 :Yb 0.5 mol% was 24,000 ph/MeV and 4.9 % at 662 keV.
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.
Cesium Hafnium Chloride (Cs2Hfl6) is a promising metal halide scintillating detector due to its excellent characteristics such as non-hygroscopicity, high light yield without doping. Scintillators plays an important role in nuclear security applications as detectors at border monitoring stations. We grew and characterized CHC crystals to be fabricated for gamma detection. Photoluminescence was performed using the Duetta Fluorescence and Absorbance Spectrometer. The energy response to Cs-137 and Co-60 reference sources was recorded for a representative sodium iodide (NaI) scintillating detector.
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.
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.
Here, the Bridgman crystal growth and scintillation properties of both undoped and Tl-doped Cs 3 Cu 2 I 5 are presented. This material is very attractive for gamma and X-ray detection applications, with a density of 4.53 g/cm 3 and effective atomic number of 51.9. Undoped Cs 3 Cu 2 I 5 had a light yield of 41,500 photons/MeV, with an energy resolution of 4.4% at 662 keV. Thallium doping at 0.5 mol % resulted in a much-improved scintillation response, in which light yield increased to 98,200 photons/MeV and energy resolution reduced to 3.3% at 662 keV. The X-ray excited emission is centered at 442 nm for the undoped and 500 nm for the Tl-doped crystals. The undoped emission is broad, typical of excitonic emission, while thallium doping results in an even broader band with features of both the undoped and thallium defect-mediated emissions.
Ultrafast scintillators are essential for next-generation radiation detection, positron emission tomography, and high-speed medical imaging. All-inorganic CsPbBr 3 perovskites are attractive candidates because of their high stopping power, and excellent optical quality, yet their long carrier lifetimes result in slow scintillation responses on the order of hundreds of nanoseconds. Here, we demonstrate that controlled over-doping with Br 2 produces CsPbBr 3.03 single crystals with sub-nanosecond scintillation at room temperature while preserving crystal quality. Single crystals grown by the Bridgman method exhibit high transparency and maintain the orthorhombic perovskite structure. Br 2 over-doping induces a slight lattice expansion (about 0.42% increase in unit-cell volume) while maintaining the orthorhombic perovskite phase and high optical transparency. Optical absorption reveals a slight redshift of the absorption edge after Br 2 introduction, indicating a modified defect landscape. Time-resolved photoluminescence and radioluminescence measurements show that Br 2 doping creates dense and efficient recombination centers that reduce the scintillation decay time from more than 100 ns in undoped crystals to 350 ps under 5.486 MeV α-particle excitation, and the scintillation decay time decreases by two orders of magnitude. The doped crystals also achieve a spatial resolution of 12 lp mm −1 in X-ray imaging. These results reveal a defect-engineering route for achieving ultrafast scintillation in halide perovskites and highlight the potential of Br 2 -modified CsPbBr 3 for fast timing applications.
The vast variety of nuclear security applications require radiation detection materials tailored to their operational needs. A scintillator’s properties are strongly influenced by the choice of luminescent dopant, which facilitates customization to different applications. In this work, transparent Ø12 mm single crystals of undoped CsCaCl 3 , CsCaCl 3 :1% Eu, CsCaCl 3 :1% Tl, and CsCaCl 3 :1% Eu, 1% Tl were grown via the Vertical Bridgman method. Their scintillation properties and fast neutron-gamma discrimination capabilities were investigated. Undoped CsCaCl 3 had a light yield of 2,500 ph/MeV, which is the highest reported to date for this CVL material. The incorporation of Eu 2+ or Tl + into CsCaCl 3 as luminescence centers resulted in significantly higher light yields of ∼16,000 ph/MeV and energy resolutions of ∼8% at 662 keV. Compared to the single dopant counterparts, CsCaCl 3 :Eu, Tl had significantly suppressed afterglow; however, this came at the cost of reduced light yield. Among the materials tested, only CsCaCl 3 :Tl showed effective fast neutron and gamma discrimination capabilities, achieving a Figure of Merit of 3.2 between gamma-rays and fast neutron captures that produce protons and 1.6 between gamma-rays and fast neutron captures that produce alpha particles.
In this study, halide perovskite nanocrystal scintillators detect high-energy protons with sensitivity suitable for clinical applications.
Scintillators play crucial roles in homeland security applications like gamma ray spectroscopy and high energy X-ray radiography. For promising new scintillators, fine-tuning the luminescent dopant concentration is one avenue to further improve their performance and tailor their properties. In this work, the effects of europium dopant concentrations on the crystal growth, luminescence and scintillation properties of RbSr 2 Br 5 and RbSr 2 I 5 crystals was investigated. Nine transparent 7 mm diameter single crystals were grown via the Vertical Bridgman method. Here, the optical band gap of RbSr 2 Br 5 was 5.9 eV and that of RbSr 2 I 5 was 4.7 eV. High scintillation performance was achieved with a relatively low europium concentration of 1 mol%. For both RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu crystals, light yield of 60–90,000 ph/MeV, energy resolution 2.8–4.0 % at 662 keV, and X-ray afterglow 0.79–1.5 % at 2 ms were obtained.
The unique optoelectronic properties of metal halide perovskite quantum dots (QDs) make them promising candidates for applications in light-emitting diodes (LEDs), scintillators, and other photonic devices. The automated micropipetting synthesis platform equipped with an optical reader enables the opportunity for high throughput synthesis and photoluminescent (PL) characterization of metal halide perovskite QDs for the first time. Here, we explore the compositional dependence of the PL behavior and stability of the combinatorial library of cesium lead halide (CsPbX 3 ) perovskites QDs via the automated platform. To study the stability of synthesized QDs in the binary and ternary configurations, we study the time-dependent PL properties using previously developed machine learning analysis. Additionally, to systematically explore the PL behavior in the ternary CsPbX 3 QDs system, we introduce the Bayesian inference framework that allows the probabilistic fit of multiple models to the PL data and establishes both optimal model and model parameter robustly. Furthermore, these behaviors can be used as a control parameter for the navigation of the multidimensional compositional spaces in automated synthesis. Furthermore, this analysis shows the nonuniformity of the PL peak behavior in the ternary CsPbX 3 QDs system. Further, the analysis confirms narrow size distribution and good quality of CsPbBr 3 QDs alloyed with low concentrations of iodide and chloride. We note that Bayesian Inference fit parameters can be further used as a control signal for navigation of the chemical spaces in automated synthesis.
A low cost, rapid, flexible radiation detector uses inorganic metal halide precursors and dyes that respond to self-quenching hybrid scintillation. Remote, high-contrast, laser sensing can be used to determine when exposure of the detector to radiation occurs (even temporally).