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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. 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The PEA2PbBr4 scintillator exhibits varied performance in photoluminescence (PL) and radioluminescence (RL) profiles. PL in the reflectivity mode shows emission peaks at 414 and 434 nm, whereas PL and RL in the transmission mode exhibit only one peak at 434 nm. Temperature-dependent PL spectra measurements confirm that self-absorption contributes to this difference. PEA2PbBr4 displays decay times of 1.3 ns (90%) and 4.4 ns (10%) for PL and 11.5 ns (89%) and 47 ns (11%) for RL. To explain the distinct decay times, we construct two models for simulating laser and radiation excitation and investigate carrier dynamics using non-adiabatic molecular dynamics. Our findings suggest that the relatively long radiative recombination process of carriers contributes to the slow RL decay time. [ABSTRACT FROM AUTHOR]

The aim of this work is to highlight the correlation between treatment conditions, composition, and structure of reduced zinc oxide (ZnO:Zn) with optical and radioluminescence properties for the production of high yield scintillating powders. Purchased zinc oxide (ZnO) powders (≈0.35 ± 0.15 μm) were thermally reduced in Ar/H2 (3%) atmosphere at temperatures ranging between 600 (≈0.40 ± 0.17 μm) and 1000 °C (≈6.4 ± 1.6 μm), obtaining ZnO:Zn powders. The reduction degree, evaluated through energy dispersive spectroscopy, showed a linear increase from 0% up to 20% (800 °C sample), reaching a plateau condition at about 25% for the highest treatment temperatures (1000 °C sample). Structural analysis highlighted the existence of a threshold temperature, previously reported in the literature, around 800 °C, beyond which (i) the grain size remarkably increases, (ii) the shape changes from hexagonal to round-shaped, and (iii) the intensity of electron spin resonance (ESR)-active defects at g = 1.9596 decreases for a new resonance at g = 2.0105. Additionally, a substantial variation, from 5.63 ± 0.02 down to 5.2 ± 0.1 g/cm3, of the skeletal density and a slight contraction of the optical bandgap are observed. Unlike the structural properties, PL and x-ray radioluminescence showed a continuous increase of the green emission intensity, associated with ESR-active ionized oxygen vacancies and ESR non-active recombination centers, and of the PL defective lifetimes (33 ns < τfast < 88 ns, 395 ns < τslow < 930 ns). [ABSTRACT FROM AUTHOR]

Phosphorescent octahedral metal cluster complexes are highly attractive in terms of biomedical applications, particularly in the area of luminescent diagnostics and photodynamic therapy (PDT). The ability of clusters to be excited by x-radiation followed by red/near infrared emission makes them a new promising class of photosensitizers for deep-PDT. This work demonstrates a direct observation of x-ray-excited optical luminescence of hexanuclear clusters, by example of rhenium cluster complex Na4[{Re6Se8}(CN)6], in a true aqueous solution. The article also describes point-by-point the details and pitfalls of studying cluster radioluminescence in aqueous solution. [ABSTRACT FROM AUTHOR]

Scintillators are key components in high-energy x-ray detectors for x-ray computed tomography, which are applied in medical diagnosis, nondestructive testing, and security inspection. Scintillators in x-ray imaging are required to have both high spatial resolution and sensitivity; however, a trade-off between spatial resolution and sensitivity exists. To improve the sensitivity of a scintillator, its thickness must be increased; however, spatial resolution deteriorates with increasing thickness. Here, we developed a well-aligned Tb-doped GdAlO3-αAl2O3 phase-separated scintillator fiber (PSSF) with a diameter of 1.25-μm by a micro-pulling-down method. The luminescence, scintillation, and imaging performances of a grown PSSF sample were evaluated. X-ray-induced radioluminescence measurements of the sample showed Tb3+ 4f–4f emissions in the wavelength range of 470–700 nm, and the maximum emission peak was at 550 nm. The contrast transfer function at 10 lp/mm was 82% for both 270 and 500 μm-thick PSSF samples. We calculated the luminescence index, which is the product of the scintillator's light yield and sensitivity, of the samples and compared their values with commercially available conventional CsI:Tl columnar scintillators. The Tb-doped GdAlO3-αAl2O3 PSSF exhibits higher contrast transfer function and luminescence index values at above 60 keV x-ray region compared with the tested conventional scintillators. [ABSTRACT FROM AUTHOR]

Optical strategies like Cerenkov luminescence imaging (CLI) or radioluminescence imaging (RLI) to image clinically available positron emission tomography and single photon emission computed tomography probes still suffer from low sensitivity or resolution. This study investigated a painted radioluminescence imaging (PRLI) approach that employed a painted scintillator to improve signal and resolution for imaging clinical used 18F-fluorinated deoxyribose (18F-FDG). Results of phantom and in vivo experiments revealed that PRLI could achieve ∼100 times higher signal intensity than CLI and higher resolution compared to Flexible radioluminescence imaging (FRLI), a flexible scintillation-based RLI. PRLI increased signal-to-background ratio in the pseudotumor model by 81.8% (compared to CLI) and 73.9% (compared to FRLI) as well as in the tumor model by 60.0% (compared to CLI) and 33.3% (compared to FRLI). As a conclusion, PRLI is a more effective optical approach for detecting tumors using 18F-FDG. [ABSTRACT FROM AUTHOR]

Cerenkov luminescence imaging (CLI) is an imaging method that uses an optical imaging scheme to probe a radioactive tracer. Application of CLI with clinically approved radioactive tracers has opened an opportunity for translating optical imaging from preclinical to clinical applications. Such translation was further improved by developing an endoscopic CLI system. However, two-dimensional endoscopic imaging cannot identify accurate depth and obtain quantitative information. Here, we present an imaging scheme to retrieve the depth and quantitative information from endoscopic Cerenkov luminescence tomography, which can also be applied for endoscopic radio-luminescence tomography. In the scheme, we first constructed a physical model for image collection, and then a mathematical model for characterizing the luminescent light propagation from tracer to the endoscopic detector. The mathematical model is a hybrid light transport model combined with the 3rd order simplified spherical harmonics approximation, diffusion, and radiosity equations to warrant accuracy and speed. The mathematical model integrates finite element discretization, regularization, and primal-dual interior-point optimization to retrieve the depth and the quantitative information of the tracer. A heterogeneous-geometry-based numerical simulation was used to explore the feasibility of the unified scheme, which demonstrated that it can provide a satisfactory balance between imaging accuracy and computational burden. [ABSTRACT FROM AUTHOR]

Temperature dependence of the luminescence characteristics of Lu1.84Y0.16SiO5:Ce (LYSO:Ce) scintillator was investigated under x-ray excitation. The luminescence decay time, light yield, radioluminescence (RL) spectra, spatial resolution, and luminescence homogeneity from 300 to 550 K are experimentally examined with multiple x-ray facilities. The results show that the decay time and light output of the LYSO:Ce scintillator will decrease from 42 to 1.89 ns and from 32 000 to 1120 photons/MeV with a temperature increase from 300 to 550 K, respectively. The RL spectrum experiments demonstrate that the spectrum peak will move from 414 to 426 nm when adjusting the temperature from 300 to 550 K. The spatial resolution experiments show that the spatial resolution is hardly affected and can reach as high as 2.5 lp/mm when increasing the temperature from 300 to 550 K, and the luminescence homogeneity remains unchanged with increase in temperature. The experimental results provide important information for the radiation imaging application of the LYSO:Ce scintillator. [ABSTRACT FROM AUTHOR]

We report the results from optical absorption, photoluminescence, radioluminescence, and optically stimulated luminescence measurements on polycrystalline NaMgF3(Mn). A point defect that absorbed near 340 nm at 300K was observed after X-ray irradiation, which is not seen in the pure compound and may be due to self-trapped holes close to the Mn sites. This defect could be optically bleached, and optically stimulated luminescence was observed during the bleaching process. Non-distorted and distorted Mn2+ photoluminescence was found where only the non-distorted sites showed optically stimulated luminescence. Both sites displayed radioluminescence, but the dependence on the radiation dose was different for each site. An F-center Mn complex was observed after X-ray irradiation, which has not been previously reported for the NaMgF3(Mn) compound. The photoluminescence emission at 670 nm from this complex increased with increasing radiation dose and was not bleached by optical excitation at 566 nm. However, it could be bleached after 254 nm excitation. Thus, unlike Mn2+ optically stimulated luminescence, the photoluminescence from this emission can be used to provide a non-destructive measure of the radiation dose. Our results show that NaMgF3(Mn) can potentially be used as a radiation dosimeter for dose-rate monitoring via radioluminescence, continual monitoring of individual doses via F-center Mn complex photoluminescence, and cumulative dose detection via optically stimulated luminescence. [ABSTRACT FROM AUTHOR]

Low energy conversion efficiency and low output power are the major limiting factors of isotope batteries as miniature power supplies for the broad applications, such as micro-electromechanical systems and aerospace electronics. In this work, highly efficient x-ray radioluminescent batteries are demonstrated based on single-crystal scintillators and spectra-matched photovoltaic batteries. X-ray sources are chosen to reduce the backscattering loss, and cerium doped Gd3Al2Ga3O12 (GAGG:Ce) single-crystal scintillators are adopted to improve the radioluminescence efficiency and light coupling efficiency, for their high x-ray absorption ability and high light-yield. The bandgap of photovoltaic battery is also optimized to match the luminescence spectrum of GAGG:Ce to maximize the photovoltaic efficiency. An optimal radioluminescent battery is achieved with an output power of 13.4 μW/cm2 and a conversion efficiency of 1.28%, which is a 10.7-times improvement in the previous best reports (0.12%). This exciting progress indicates the promising potential of radioluminescent batteries in broad applications and will inspire the further exploration for the research community of radioisotope batteries. [ABSTRACT FROM AUTHOR]

Low temperature radioluminescence and thermoluminescence spectra of ZnO track numerous changes produced by copper ion implantation into the surface layer. A significant, but unexpected, feature is that the bulk crystal becomes modified by the stress generated in the surface layer. This is reflected by the energy of intrinsic band gap emission. There are also differences in the spectra and peak temperatures of the thermoluminescence components, consistent with such a structural relaxation. The copper implant layer is both absorbing and reflective, so this introduces major distortions on the radioluminescence component from the bulk region, since the bulk luminescence signals are transmitted through, or reflected from, the implant layer. The temperature dependence of the spectra includes anomalies that are typical of changes driven by phase transitions of nanoparticle inclusions. Overall, the features of bulk relaxation, spectral distortion, and detection of nanoparticle inclusions are rarely considered for ion implanted luminescence studies, but the data suggest they are almost inevitable in a wide range of implanted materials. [ABSTRACT FROM AUTHOR]

Systematic characterization of semiconductor colloidal quantum dots (cQDs) response to ionizing radiation must be performed to use them in radiation detection. In this study, the robustness of multi-shell (MS) and core/shell (CS) cQDs was investigated under irradiation. Radioluminescence (RL) measurements with kV and MV photon beams revealed a better resistance of MS cQDs to ionizing radiation, with their spectra fluctuating by barely ~ 1 nm. A systematic signal recovery between subsequent irradiations was noticed for MS cQDs only. A beam energy dependence of the RL stability was detected between kV and MV energies. At the same point of dose cumulated, the RL signal loss for the kV beams was observed to be ~6-7% smaller than that of the MV beam, for both types of cQDs. These results demonstrate that MS cQDs are better candidates as ionizing radiation sensors than CS cQDs, especially in the kV energy range. [ABSTRACT FROM AUTHOR]

Our previous study showed a great attenuation for the Cerenkov luminescence endoscope (CLE), resulting in relatively low detection sensitivity of radiotracers. Here, a kind of radioluminescence nanoparticles (RLNPs), terbium doped Gd2O2S was mixed with the radionuclide 68Ga to enhance the intensity of emitted luminescence, which finally improved the detection sensitivity of the CLE by using the radioluminescence imaging technique. With the in vitro and in vivo pseudotumor experiments, we showed that the use of RLNPs mixed with the radionuclide 68Ga enabled superior sensitivity compared with the radionuclide 68Ga only, with 50-fold improvement on detection sensitivity, which guaranteed meeting the demands of the clinical diagnosis of gastrointestinal tract tumors. [ABSTRACT FROM AUTHOR]

Radio-luminescence (RL) optical fiber sensors enable a remote, punctual, and real time detection of ionizing radiation. However, the employment of such systems for monitoring extended radiation fields with energies above the Cerenkov threshold is still challenging, since a spurious luminescence, namely, the "stem effect," is also generated in the passive fiber portion exposed to radiation. Here, we present experimental measurements on Yb-doped silica optical fibers irradiated with photon fields of different energies and sizes. The results demonstrate that the RL of Yb3+, displaying a sharp emission line at about 975 nm, is free from any spectral superposition with the spurious luminescence. This aspect, in addition with the suitable linearity, reproducibility, and sensitivity properties of the Yb-doped fibers, paves the way to their use in applications where an efficient stem effect removal is required. [ABSTRACT FROM AUTHOR]