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In this study, we demonstrated a drastic improvement in energy resolution of (Lu0.75Y0.25)3Al5O12:Pr (LuYAG) single crystal scintillators from 4.8% to 4.1% at 662 keV upon Li+ codoping, which is the best value ever reported in the class of oxide single crystal scintillators. Li+ codoping can also significantly enhance its scintillation yield from 16 000 to 25 000 photons MeV−1, but slightly prolong the scintillation decay time. As Li+ codoping was found to have a negligible effect on the light yield non‐proportionality, we attributed the significant improvement in energy resolution to the reduced statistical variance in the number of photoelectrons produced in the photomultiplier tube (Rstat). [ABSTRACT FROM AUTHOR]

Organic–inorganic and all-inorganic halide perovskites have become leading candidates toward high-performance optoelectronic devices and radiation detectors. In this work, we report novel zero-dimensional Cs4EuX6 (X = Br, I) perovskite single crystals as self-activated scintillators with superior performance for gamma-ray spectroscopy. Both Cs4EuBr6 and Cs4EuI6 single crystals grown by the Bridgman method were determined to have the trigonal crystal structure with the R3̅c space group, and have a melting point of approximately 540 °C. Cs4EuBr6 and Cs4EuI6 exhibit blue emission under UV excitation and high light yields of 78 000 ± 4000 photons per MeV and 53 000 ± 3000 photons per MeV under 137Cs gamma-ray irradiation, respectively. In particular, the former represents the best result achieved for self-activated scintillators thus far. Thermally stimulated luminescence studies and density functional theory calculations elucidate the correlation between halogen vacancies and long-lived emission (afterglow) at room temperature in Cs4EuX6 (X = Br, I) single crystals. Our findings not only demonstrate the high gamma-ray detection efficiency in Cs4EuX6 (X = Br, I), but will further promote the development of 0D metal halide-based novel luminescent and radiation detection materials. [ABSTRACT FROM AUTHOR]

Codoping is an effective approach for precise control of point defects in many advanced materials, and can be used to optimize their function. This paper reports an effort toward tailoring the scintillation properties of metal halides through defect engineering. A study of aliovalent codoping of the KCaI3:Eu2+ single‐crystalline scintillators is performed, through which it is discovered that a simultaneous suppression of X‐ray induced afterglow and improvement of gamma‐ray energy resolution can be successfully achieved via Zr4+ codoping. The afterglow level is reduced by more than twofold with Zr4+ codoping. The energy resolution of a 5 mm cubic KCaI3:Eu2+ sample is improved from 3.25 to 2.7% at 662 keV, and 6.5 to 5.73% at 122 keV upon Zr4+ codoping. Physical explanations for the improvements are revealed from our investigations into both the electronic structure and thermodynamics of the defects by using thermoluminescence techniques and density functional theory calculations. The codoped Zr4+ ions prefer to form interstitials acting as shallow electron traps. The {ZrCa+VCa} complex can co‐exist with Zri interstitials as shallow hole traps under certain condition, which are able to trap holes temporarily. [ABSTRACT FROM AUTHOR]

A quaternary iodide KCa0.8Sr0.2I3:Eu2+ scintillator with 2.5% energy resolution at 662 keV in a 5 mm3 sample shows great potential for use in gamma-ray spectroscopy applications. In this work, we report the state-of-the-art growth of high quality 25, 38, and 50 mm diameter KCa0.8Sr0.2I3:Eu2+ single crystals by the vertical self-seeding Bridgman method. KCa0.8Sr0.2I3:Eu2+ with a size of ∅25 mm × 25 mm can achieve excellent energy resolutions of 3.15% at 662 keV and 6.8% at 122 keV irradiation, which are superior to that of a commercial NaI:Tl+ of the same size. The nonuniformity of light collection and production in ∅25 mm × 25 mm and ∅38 mm × 38 mm KCa0.8Sr0.2I3:Eu2+ crystals was evaluated by using a technique based on a collimated 137Cs source and coupling the crystal to a photomultiplier tube (PMT) in different directions. The performances of the packaged crystals for practical use were also measured. [ABSTRACT FROM AUTHOR]

Ternary halide scintillators are commonly prepared from a mixture of commercially available binary halides. The initial binary halides may contain excess halogen ions or have different volatilities, which could lead to loss of stoichiometry of the resulting ternary halide crystals and potentially negatively affect optical and scintillation properties. In this work, the effects of vacuum aging of the melt (melt aging) and use of off-stoichiometric melts via introduction of excess CsI on the crystal quality and scintillation properties of CsSrI3:Eu2+, a promising scintillator for gamma-ray detection applications, are investigated. The phase purity of the grown samples was confirmed by powder X-ray diffraction and differential scanning calorimeter measurements, and the existence of matrix composition variations is revealed by energy-dispersive X-ray spectroscopy analyses. An abnormal relationship between the full energy peak and the shaping time, i.e. full energy peak broadening or existence of two full energy peaks, in the melt-aged and off-stoichiometric samples is observed. It is ascribed to a slow scintillation decay event in a time scale between 15 and 50 μs. For the CsSrI3:Eu2+ single crystal grown from a stoichiometric melt without melt aging treatment, an energy resolution of 5.0% at 662 keV and a light yield of 48 000 ± 2000 photons per MeV can be achieved at a size of 1.4 cm3. [ABSTRACT FROM AUTHOR]

GGAG:Ce crystals with various Ca concentrations were grown by the Czochralski technique. The introduction of Ca2+ ions into a trivalent site results in a change in the Ce valence state as well as an additional F+ luminescence center. The changes of Ce valence state could be affected by various annealing atmospheres and were investigated via measuring the Ce3+ absorbance and observing the color change of the sample. Photoluminescence spectra and photoluminescence decay were used to reveal the occurrence of F+ center related to the oxygen vacancies during the annealing. A redox mechanism and a charge compensation process are proposed to explain the change in Ce state charge and F+ center during the annealing. [ABSTRACT FROM AUTHOR]

Single crystals of Gd_3Ga_3A l_2O12:Ce with Ca, B and Ba codopants were successfully grown using the Czochralski technique. The samples of each composition were irradiated to 10 kGy and 100 kGy gamma dose to determine the radiation induced absorption. The Ca co-doped crystal was found to have maximum induced absorption, while B and Ba co-doped were found to be more radiation hard. The reduction in transmission could be partially restored at room temperature without any annealing treatment of the crystals. The additional absorption was also measured after annealing the crystals in reducing environment and compared with the radiation induced absorption. Thermoluminescence measurements were carried out to explain the defect structure and recovery of the transmission reduction at room temperature. [ABSTRACT FROM PUBLISHER]

The temperature dependence of scintillation decay and rise time was measured for GGAG:Ce and Ca-codoped GGAG:Ce crystals in the temperature range of 10 K to 400 K. The decay and rise times were found to increase with decreasing temperature in the case of GGAG:Ce crystals, while Ca codoping modifies the kinetics such that decay and rise times are constant with the change in temperature. In order to obtain a better understanding of the role of trap centers in the temperature dependence of scintillation kinetics, spectrally resolved thermoluminescence (TL) properties were also studied for these crystals. [ABSTRACT FROM PUBLISHER]

The temperature dependence of the photoluminescence properties of Gd2SiO5:Ce,Ca crystals was found to be significantly affected by Ca codoping and shows that presence of additional energy levels in these crystals provides nonradiative energy transfer. The excitation and emission bands also broaden with codoping due to presence of these additional energy levels. Therefore Ca codoping in Gd2SiO5 crystals decreases the scintillation decay very strongly and has a strong adverse affect on scintillation light yield, different from the effect in other members of the oxyorthosilicate family such as Lu2SiO5 and Y2SiO5. [ABSTRACT FROM PUBLISHER]

Experimental studies of LSO:Ce crystals co-doped with various concentrations of Ca are presented. Photoluminescence decay time, excitation and emission spectra, thermal response and X-ray excited luminescence are investigated as a function of Ca concentration. Experimental data show Ca co-doping does not alter the energy level structure of either Ce1 or Ce2, but reduces the relative population of Ce2 to Ce1. Thus, the luminescence from Ce2 is suppressed, which contributes to the fast scintillation decay of Ca co-doped LSO:Ce. [ABSTRACT FROM AUTHOR]

Low temperature (∼35 K) measurements of the scintillation kinetics of Y2SiO5 : Ce (YSO:Ce) have previously illustrated that shallow electron traps can play an important role in the scintillation mechanism. In addition, divalent calcium co-doping of isostructural Lu2SiO5 : Ce (LSO:Ce) has been shown to eliminate shallow electron traps and decrease scintillation decay time while maintaining high light output. Here we investigate the effect of Ca2+ codoping on the trap populations and scintillation kinetics of YSO:Ce. Single crystals were grown with Ca2+ concentrations up to 0.5 at% relative to Y. Thermoluminescence measurements indicate a significant reduction in shallow traps, and a marked change in the scintillation kinetics can be seen in the scintillation time profiles as a result of Ca2+ codoping. [ABSTRACT FROM AUTHOR]

Commercially available Lu2SiO5:Ce (LSO:Ce) scintillators for the nuclear medical imaging applications, such as positron electron tomography (PET), normally have a light yield of 30 000–32 000 photons/MeV and a scintillation decay time of 43–45 ns. We demonstrate a simultaneous improvement of light yield and decay time of LSO:Ce single crystal scintillators with lithium codoping. Li codoping significantly enhances the light yield of LSO:Ce from 32 500 to 39 000 photons/MeV, shortens the scintillation decay time from 45.4 to 42.1 ns, and reduces the room temperature afterglow by around one order of magnitude. The physical insights on the role of Li codopants in scintillation mechanism are provided by studying cerium oxidation state, luminescence properties of cerium activator centers, defect structure, and preferential occupation of lithium ions. The improved light yield and afterglow are explained in terms of the dissociation of spatially correlated oxygen vacancies (VO) and Ce centers or the suppression of VO formation, allowing a more efficient electron migration to Ce centers. We attribute the decay time shortening upon Li+ codoping to the reduction of slow Ce2 emissions via a non‐radiative energy transfer from six‐coordinated Ce2 to seven‐coordinated Ce1 centers. This letter reports a simultaneous improvement of light yield, decay time, and afterglow of Lu2SiO5:Ce3+ scintillation detectors by Li+ codoping. Analysis reveals the non‐conversion of stable Ce3+ to Ce4+ upon Li codoping, and the critical role of Li site occupancy on the suppression of oxygen vacancies. This strategy is also expected to be extended to other oxide scintillators. [ABSTRACT FROM AUTHOR]