High Light Yield Research Articles

Characterization of plastic scintillator samples produced by a university-SME Collaboration

Scintillator samples are synthesized by a university-SME collaboration and the light yield, light emission and light transmission properties are studied with the aim of determining the fluor content that gives the highest light yield. Three plastic scintillator samples with different fluor additives are produced and their optical properties are found to be comparable with a high-light-yield EJ-204 reference sample. Amongst the three, the sample with 0.75% PPO + 0.75 %PTP and 0.04% POPOP + 0.04% Bis-MSB provides the highest light yield. The authors plan to use the same fluor additive concentration to produce application-specific scintillators that are not commercially available for nuclear reactor monitoring and medical applications.

Synthesis of cerium-doped gadolinium gallium aluminum garnet (GGAG:Ce) scintillating powder via solvothermal method

The powder material Gd3Ga3Al2O12:Ce (GGAG doped with Cerium) has garnered significant attention in radiation detection due to its high light yield and rapid decay time. Despite its potential, the synthesis of high-quality and reproducible GGAG:Ce scintillating powder remains a considerable challenge. In this study, we present a solvothermal approach with an annealing temperature of 1300 °C for producing cerium-doped GGAG powder with varying concentrations (4, 2, and 0.5 mol%). The structural and luminescent characteristics were meticulously examined using X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), photoluminescence (PL), radioluminescence (RL) spectroscopy, and X-ray photoelectron spectroscopy (XPS). XRD analysis confirmed the single-cubic phase garnet structure of the synthesized powder. By comparing the intermediate solvothermal products synthesized at different sintering temperatures (900 °C for 3 h and 1300 °C for 1 and 3 h), a direct correlation between solvothermal conditions and the structure/property relationships of the product was established. FESEM images revealed an ellipsoidal to irregular morphology of the as-synthesized GGAG:Ce microparticles, ranging from 0.1 to 0.3 μm, regardless of the Ce concentration. PL spectra demonstrated a strong emission peak at approximately 550 nm, characteristic of Ce3+ ions. RL data confirmed the peak luminescence at around 550 nm, with an almost twofold increase in intensity as the concentration of Ce3+ increased from 0.5 mol% to 4 mol%. XPS data disclosed the Ce3+/Ce4+ ratio in solvothermally synthesized GGAG:Ce, wherein Ce loading of 4 mol% demonstrated the increase in Ce3+ concentration to 95%, whereas the concentration of Ce4+ decreased to 5%. Notably, the highest luminescence efficiency was achieved with GGAG:Ce at a 4 mol% concentration. Thus, the solvothermal method employed in GGAG:Ce synthesis presents a straightforward approach, yielding rapid results with precise control over particle morphology and size.

High‐Temperature X‐Ray Imaging with Transparent Ceramics Scintillators

AbstractScintillators with high spatial‐resolution and high‐stability are highly desirable for X‐ray imaging applications at unpredictable environments. To challenge state‐of‐the‐art technology, it is necessary to design high thermal stable scintillators with high‐resolution and high light yield. In this work, the zero‐thermal‐quenching Lu3Al5O12:Ce3+ (LuAG: Ce3+) transparent ceramics (TCs) is synthesized with high optical transparency. The thermoluminescence (TL) curves of the as‐obtained TCs demonstrate that the formation of the oxygen vacancies, acting as the trapping centers, can capture the carriers and then contribute to the enhancement of its thermals stability via the thermal compensation effect. The exceptional thermal‐stability of the TCs scintillator endows the monitoring of the dynamic changes of the internal structure of the objective samples without any ghosting effects during heating. In addition, given the ultra‐high uniform, transparency, and fast light decay of the TCs scintillator, the excellent spatial resolution (≈112 lp mm−1) of the X‐ray microscopic imaging is realized. These results undeniably demonstrate that the as‐obtained LuAG: Ce3+ TCs have great prospects for advancement in X‐ray detectors.

Organic-Inorganic Hybrid Glasses of Atomically Precise Nanoclusters.

Organic-inorganic atomically precise nanoclusters provide indispensable building blocks for establishing structure-property links in hybrid condensed matter. However, robust glasses of ligand-protected nanocluster solids have yet to be demonstrated. Herein, we show [Cu4I4(PR3)4] cubane nanoclusters coordinated by phosphine ligands (PR3) form robust melt-quenched glasses in air with reversible crystal-liquid-glass transitions. Protective phosphine ligands critically influence the glass formation mechanism, modulating the glasses' physical properties. A hybrid glass utilizing ethyldiphenylphosphine-based nanoclusters, [Cu4I4(PPh2Et)4], exhibits superb optical properties, including >90% transmission in both visible and near-infrared wavelengths, negligible self-absorption, near-unity quantum yield, and high light yield. Experimental and theoretical analyses demonstrate the structural integrity of the [Cu4I4(PPh2Et)4] nanocluster, i.e., iodine-bridged tetranuclear cubane, has been fully preserved in the glass state. The strong internanocluster CH-π interactions found in the [Cu4I4(PPh2Et)4] glass and subsequently reduced structural vibration account for its enhanced luminescence properties. Moreover, this highly transparent glass enables performant X-ray imaging and low-loss waveguiding in fibers drawn above the glass transition. The discovery of "nanocluster glass" opens avenues for unraveling glass formation mechanisms and designing novel luminescent glasses of well-defined building blocks for advanced photonics.

Measurement of nanocomposite scintillators by terahertz time domain spectroscopy.

Nanocomposite scintillators are expected to combine the advantages of inorganic and plastic scintillators, such as high detection efficiency, high light yield, fast decay time, low cost, and ease of processing. They are currently the forefront and hot field of scintillator research. In this study, a non-destructive method was developed for measuring the content of inorganic components in nanocomposite scintillators by terahertz time-domain spectroscopy. The complex refractive index of B a F 2 nanocomposite scintillators with different mass contents was measured in the terahertz band. As the mass content of B a F 2 nanoparticles increases, the refractive index and extinction coefficient of B a F 2 nanocomposite scintillators also gradually increase in the terahertz band. By combining the effective medium theory, the expected mass content was obtained, proving the feasibility of this measuring method.

Field tests for performance evaluation of a new spent-fuel verification system in heavy water reactor

The optical fiber-based measurement system has been utilized for inspecting CANDU-type spent fuel at the Wolsung site in South Korea under the nuclear safeguards of the International Atomic Energy Agency (IAEA). In our previous studies, we developed a new spent-fuel verification system to address issues of the existing instrument. While our prior work primarily focused on equipment development, we had not yet conducted comprehensive field tests to assess its performance. Recently, we conducted field tests at the Wolsung Unit 4 to thoroughly evaluate the newly developed spent-fuel verification system's performance. This paper discusses the results of these field tests, with a focus on signal sensitivity, the system's capability to distinguish neighboring spent-fuel bundles, and the optical fiber background signals. Additionally, we conducted experiments to assess how different scintillation materials impact the system's performance, including p-terphenyl organic scintillator, PVT plastic scintillator, and lithium glass scintillator. The experimental results demonstrated that the new instrument equipped with the p-terphenyl organic scintillator outperformed the existing system. The p-terphenyl scintillator emerged as the superior choice among the three radiation scintillators. Signals that were previously undetectable using the Li glass scintillator were observed in the signals obtained with the p-terphenyl and PVT plastic scintillators. The remarkable performance of the new verification instrument is attributed mainly to the p-terphenyl's high light output and low decay time. The newly developed verification system is expected to streamline IAEA safeguards inspection efforts, reducing both time and the burden on nuclear operators. This report represents the first successful application of the p-terphenyl scintillator as a radiation detector in a wet spent fuel pool. The experimental findings presented in this paper are anticipated to be valuable for researchers working on radiation detectors suitable for high radiation environments in water.

Fast Emitting Nanocomposites for High‐Resolution ToF‐PET Imaging Based on Multicomponent Scintillators

AbstractTime‐of‐Flight Positron Emission Tomography (ToF‐PET) is a medical imaging technique, based on the detection of two back‐to‐back γ‐photons generated from radiotracers injected into the body. Its limit is the ability of employed scintillation detectors to discriminate in time the arrival of γ‐pairs, that is, the coincidence time resolution (CTR). A CTR < 50 ps will enable fast imaging with ultralow radiotracer dose. Monolithic materials do not have simultaneously the required high light output and fast emission characteristics, thus the concept of scintillating heterostructure is proposed, where the device is made of a dense scintillator coupled to a fast‐emitting light material. Here a composite polymeric scintillator loaded with hafnium oxide nanoparticles is presented. This enhanced by +300% its scintillation yield, by surpassing commercial plastic scintillators. The nanocomposite is coupled to bismuth germanate oxide (BGO) realizing a multilayer metascintillator. The energy sharing between its components is observed, which activates the nanocomposite's fast emission enabling a net CTR improvement of 25% with respect to monolithic BGO. These results demonstrate that a controlled loading with dense nanomaterials is an excellent strategy to enhance the performance of polymeric scintillators for their use in advanced radiation detection and imaging technologies.

Turning self-trapped exciton emission via Sb3+ doping in zero-dimensional hybrid indium chloride for X-ray scintillation

Zero-dimensional (0D) hybrid indium halides have recently received great attention for their potential as X-ray scintillators due to their non-toxicity, superior optical properties and exceptional stability. However, most indium halides suffer from low emission efficiency, resulting in inferior performance. Herein, we demonstrate that a small amount of Sb3+ doping can greatly enhance the photoluminescence efficiency of a 0D hybrid indium chloride, DMA4InCl7. The pristine crystals exhibit weak self-trapped exciton (STE) emission centered at 620 nm with a low quantum yield of 11%. After Sb3+ doping, the STE emission efficiency can be greatly increased to 91%. The spectroscopic experiments and theoretical calculations indicate the efficient energy transfer from excited Sb3+ ions to the emitting STE state of the host is responsible for the substantial increase in emission efficiency. Furthermore, we find the energy transfer efficiency is related to the distance between dopants and [InCl6]3- units. The strong STE emission endows the doped samples with desirable X-ray scintillation performance, with a high light yield of 23500 photons/MeV and a low detection limit of 175 nGyair·s−1.

Heterovalent Co‐Doped LiLuF4 Composite Flexible Films as Persistent Luminescence Scintillator for X‐Ray High‐Resolution Extension Imaging

AbstractScintillators with high light yield, spatial resolution, and detection sensitivity are desirable for X‐ray imaging. Howerer, it remains challenging to improve the light yield and radiation detection capability of alkali metal rare‐earth fluoride (ALnF4). Herein, a type of Cu2+ ion heterovalent co‐doped LiLuF4:Tb,Cu microcrystalline scintillation material with high light yield, persistent, and thermostimulated luminescence is obtained by defect engineering. The heterovalent codoping strategy not only increases the radioluminescence (RL) intensity, but also introduces more carrier traps in the material to enhance the long‐afterglow and thermoluminescence intensity of LiLuF4:Tb microcrystals. After doping of 3 mol% Cu2+ ions, the RL efficiency is increased by 88.61%, and the X‐ray detection limit of LiLuF4:Tb,Cu reaches 2.7928 nGy·s‒1. This detectivity is considerably lower than the medical imaging requirements (5.5 µGy·s‒1). Furthermore, a large‐area flexible scintillation film of dimensions 30 × 30 cm2 is prepared to achieve high spatial resolution X‐ray imaging of 22 LP mm−1@MTF(modulation transfer function) = 0.2. Besides, this flexible film enables X‐ray imaging of curved objects and stores optical information for >48 h. This work provides a paradigm for improving the RL intensity and X‐ray detection sensitivity of alkali rare‐earth fluorides by crystal defect engineering, and enriches X‐ray high resolution extended imaging applications.

White emission metal halides for flexible and transparent x-ray scintillators

Flat-panel x-ray scintillators with a high spatial resolution at a low radiation dose rate are desirable for efficient imaging applications in medical diagnostics, security inspection, and nondestructive inspection. To promote the progress of x-ray imaging technologies, it is of great interest to explore transparent scintillators with reduced light scattering, high light yields, and uniform radioluminescence. Herein, we design and prepare a novel lead-free (C12H28N)2Cu2I4 metal halide featuring a high luminescent efficiency and white emission benefiting from the double self-trapped exciton mechanism, which enable to not only match the response of semiconductor-based sensors but also enhance light yields and decrease exposed doses to objects. Furthermore, transparent, and flexible scintillators with large areas of 20.25 cm2 demonstrate an outstanding scintillation performance including a high spatial resolution of 19.8 lp mm−1 and an ultralow detection limit of 28.39 nGyair s−1, which are ∼4 times higher and 194 times lower than typical values for medical imaging, respectively. This work provides not only a new route to explore promising alternatives with broadband emission but also a novel opportunity to develop flexible x-ray imaging technology.

Transparent and Planar Cs3Cu2Cl5 Crystals for Micrometer-Resolution X-ray Imaging Screen.

Copper-based (I) halide perovskites have emerged as a promising candidate for scintillation screens in X-ray inspection and imaging areas due to their solution processability and high light yield. Here, a centimeter-sized Cs3Cu2Cl5 single crystal was grown by a slow-cooling method. The planar orientation was controlled in a space-confined chamber, generating a planar crystal which is readily used for a scintillation screen without any further shaping. The crystal exhibited a unity photoluminescence quantum yield and superior scintillation performance. The Cs3Cu2Cl5 single crystal exhibited a high light yield up to 95,000 photons/MeV, which enabled an X-ray detector of a detection limit down to 2.7 μGyair/s. The homemade imager demonstrated a spatial resolution of 105 lp/mm, representing an unprecedented micrometer resolution in laboratory. Importantly, the stability of Cs3Cu2Cl5 was significantly improved by a new surface passivation procedure, whereby the passivated crystal reserved its phase after 6 months' storage in a vial. This work introduced a new solution-based synthetic method for two-dimensional scintillating crystals, opening many avenues to high-performance X-ray imaging applications.

Thermally Activated Delayed Fluorescence (TADF)-active Coinage-metal Sulfide Clusters for High-resolution X-ray Imaging.

The study of facile-synthesis and low-cost X-ray scintillators with high light yield, low detection limit and high X-ray imaging resolution plays a vital role in medical and industrial imaging fields. However, the optimal balance between X-ray absorption, decay lifetime and excitonic utilization efficiency of scintillators to achieve high-resolution imaging is extremely difficult due to the inherent contradiction. Here two thermally activated delayed fluorescence (TADF)-actived coinage-metal clusters M6 S6 L6 (M=Ag or Cu) were synthesized by simple solvothermal reaction, where the cooperation of heavy atom-rich character and TADF mechanism supports strong X-ray absorption and rapid luminescent collection of excitons. Excitingly, Ag6 S6 L6 (SC-Ag) displays a high photoluminescence quantum yield of 91.6 % and scintillating light yield of 17420 photons MeV-1 , as well as a low detection limit of 208.65 nGy s-1 that is 26 times lower than the medical standard (5.5 μGy s-1 ). More importantly, a high X-ray imaging resolution of 16 lp/mm based on SC-Ag screen is demonstrated. Besides, rigid core skeleton reinforced by metallophilicity endows clusters M6 S6 L6 strong resistance to humidity and radiation. This work provides a new view for the design of efficient scintillators and opens the research door for silver clusters in scintillation application.

Thermally Activated Delayed Fluorescence (TADF)‐active Coinage‐metal Sulfide Clusters for High‐resolution X‐ray Imaging

AbstractThe study of facile‐synthesis and low‐cost X‐ray scintillators with high light yield, low detection limit and high X‐ray imaging resolution plays a vital role in medical and industrial imaging fields. However, the optimal balance between X‐ray absorption, decay lifetime and excitonic utilization efficiency of scintillators to achieve high‐resolution imaging is extremely difficult due to the inherent contradiction. Here two thermally activated delayed fluorescence (TADF)‐actived coinage‐metal clusters M6S6L6 (M=Ag or Cu) were synthesized by simple solvothermal reaction, where the cooperation of heavy atom‐rich character and TADF mechanism supports strong X‐ray absorption and rapid luminescent collection of excitons. Excitingly, Ag6S6L6 (SC‐Ag) displays a high photoluminescence quantum yield of 91.6 % and scintillating light yield of 17420 photons MeV−1, as well as a low detection limit of 208.65 nGy s−1 that is 26 times lower than the medical standard (5.5 μGy s−1). More importantly, a high X‐ray imaging resolution of 16 lp/mm based on SC‐Ag screen is demonstrated. Besides, rigid core skeleton reinforced by metallophilicity endows clusters M6S6L6 strong resistance to humidity and radiation. This work provides a new view for the design of efficient scintillators and opens the research door for silver clusters in scintillation application.

Real-time single-proton counting with transmissive perovskite nanocrystal scintillators

High-sensitivity radiation detectors for energetic particles are essential for advanced applications in particle physics, astronomy and cancer therapy. Current particle detectors use bulk crystals, and thin-film organic scintillators have low light yields and limited radiation tolerance. Here we present transmissive thin scintillators made from CsPbBr3 nanocrystals, designed for real-time single-proton counting. These perovskite scintillators exhibit exceptional sensitivity, with a high light yield (~100,000 photons per MeV) when subjected to proton beams. This enhanced sensitivity is attributed to radiative emission from biexcitons generated through proton-induced upconversion and impact ionization. These scintillators can detect as few as seven protons per second, a sensitivity level far below the rates encountered in clinical settings. The combination of rapid response (~336 ps) and pronounced ionostability enables diverse applications, including single-proton tracing, patterned irradiation and super-resolution proton imaging. These advancements have the potential to improve proton dosimetry in proton therapy and radiography.

Effect of optimized quaternary waveguides on the performance of deep ultraviolet laser diodes

Efficient ultraviolet (UV) laser diodes (LD) emitting in the 260–270 nm range have been proposed numerically in this work. Using engineered quaternary waveguides (QWGs) in place of conventional ternary waveguides, in the p-region, results in much higher output power as well as internal quantum efficiency (IQE) and lower the lasing threshold. The electron outflow is reduced and the injection of holes is enhanced which results in high efficiency and high light power output.

Scintillation properties of lithium-6 salicylate-loaded liquid scintillators.

The limited availability of conventional 3He proportional counters provides impetus for developing novel neutron detectors. As a candidate, lithium-6-loaded liquid scintillators with neutron/gamma pulse shape discrimination (n-γ PSD) capabilities have been developed. However, the trade-off relationship between the 6Li-loading amount and scintillation light yield is a significant problem. This is because 6Li-loading involves the addition of non-luminescent materials, which cause non-radiative relaxation of the excited states. Therefore, aiming to reduce non-radiative relaxation, we chose lithium-6 salicylate (6LiSal), which shows fluorescence in the visible light region, as a chemical for 6Li-loading. In this study, we analyzed the photoluminescence/scintillation properties based on the Förster resonance energy transfer and investigated the optimal content for obtaining a high light yield. By maximizing the sequential energy transfer from the solvent (toluene) to the phosphor (POPOP), a high light yield 6Li-loaded liquid scintillator (4220 photons per MeV under gamma-ray irradiation) with a 6Li concentration of approximately 0.1 wt% was developed. Thermal neutron events were successfully detected with a light yield of 3970 photons per neutron, which is more than three times higher than those of other organic scintillators. In addition, focusing on the triplet-triplet annihilation process and further optimizing the component for the n-γ PSD, the thermal neutron and gamma-ray events were successfully separated. The developed high light yield 6Li-loaded liquid scintillators show n-γ PSD capabilities and can be promising candidates as alternative detectors to the 3He proportional counter.

Yellow-emissive organic copper(i) halide single crystals with [Cu4I4] cubane unit as efficient X-ray scintillators

The (4-bzpy)4Cu4I4 compound exhibits excellent X-ray scintillation properties with a high light yield and great potential in X-ray imaging applications.

Robust Organogel Scintillator for Self-healing and Ultra-flexible X-ray Imaging.

Metal halide scintillators serve as promising candidates for X-ray detection due to their high attenuation coefficients, high light yields, and low-cost solution-processable characteristics. However, the issues of humidity/thermal quenching and mechanical fragility, remain obstacles to the broad and diversified development of metal halide scintillators. Here, this work reports a lead-free, water-stable, stretchable, and self-healing (ethylenebis-triphenylphosphonium manganese (II) bromide (C38H34P2)MnBr4 organogel scintillator that meets X-ray imaging in complex scenarios. The robust organogel scintillator can be stretched with elongation up to 1300% while maintaining the scintillation properties. Activated by the dynamic hydrogen bonds and coordination bonds design, the organogel scintillator exhibits excellent self-healing properties at room temperature to alleviate the vignetting problem of the rigid scintillator films, the X-ray imaging resolution can reach 16.7 lp mm-1. The organogel scintillator can also realize flexible and self-healing X-ray imaging in water, providing a design path for portable devices in harsh conditions.

Multiple Energy Transfer Channels in Rare Earth Doped Multi-Exciton Emissive Perovskites.

Revealing the energy transfer (ET) process from excitons to rare earth ions in halide perovskites has great guiding value for designing optoelectronic materials. Here, the multiple ET channels in multi-exciton emissive Sb3+ /Nd3+ co-doped Cs2 ZrCl6 are explored to comprehend the ET processes. Förster-Dexter ET theory reveals that the sensitizer concentration rather than the overlap integral of the spectra plays the leading function in the comparison of the ET efficiency among multiple ET channels from the host self-trapped excitons (STEs) and dopant triplet STEs to Nd3+ ions. Besides, Sb3+ /Nd3+ co-doped Cs2 ZrCl6 enables varied color delivery and has great potential as anti-counterfeiting material. Under X-ray irradiation, Sb3+ /Nd3+ co-doped Cs2 ZrCl6 presents a high light yield of ≈13300 photons MeV-1 and promising X-ray imaging ability. This work provides new insight for investigating the ET efficiency among multiple ET processes and presents great potentiality of multi-exciton emissive perovskites in the fields of anti-counterfeiting and X-ray imaging.

Scintillation Performance of Mn(II)‐Doped Cs2NaBiCl6 Double Perovskite Nanocrystals for X‐Ray Imaging Applications

AbstractLead‐free halide perovskite‐based X‐ray scintillators with high light yield (LY) and low detection limit (LOD) have become a growing subject of research interest due to their promising application in a wide range of areas, from security to healthcare. Herein, a modified hot injection method is employed to synthesize Mn(II)‐doped Cs2NaBiCl6 double perovskite nanocrystals (DPNCs) and to examine their scintillating properties for application in X‐ray imaging and detection. The Mn(II)‐doped Cs2NaBiCl6 DPNCs exhibit a broad orange photoluminescence (PL) band at 586 nm with a PL quantum yield of 10.6%, attributed to the 4T2g(4G) → 6A1g(6S) transition of Mn2+. Temperature‐dependent PL and time‐resolved PL spectra of 4.04% Mn(II)‐doped Cs2NaBiCl6 demonstrate that the orange emission intensity initially reaches a maximum and subsequently decreases, while the decay lifetimes monotonically decrease with increasing temperature. This inconsistency can be due to the effect of the [MnCl6]4− octahedra and electron‐phonon coupling at elevated temperatures. Further, 0.05 mm thick Cs2NaBiCl6:4.04%Mn@poly(methyl methacrylate) scintillator film is synthesized with an LY of 28,350 photons MeV−1 and a LOD of 45.2 nGyair s−1. Additionally, this film demonstrates good X‐ray imaging performance with a spatial resolution of 14.76 line pairs (lp) mm−1 and shows exceptional stability under prolonged X‐ray exposure.