Luminescence properties of Y3Al5O12:Ce nanoceramics

Comparative analysis of the luminescent properties of Y₃Al₅O₁₂:Ce (YAG:Ce) transparent optical ceramics (OС) with those of single crystal (SC) and single crystalline film (SCF) analogues has been performed under excitation by pulsed synchrotron radiation in the fundamental absorption range of YAG host. It has been shown that the properties of YAG:Ce OC are closer to the properties of the SCF counterpart, where Y_Al antisite defects are completely absent, rather than to the properties of SC of this garnet with large concentration of Y_Al antisite defects. At the same time, the luminescence spectra of YAG:Ce OC show weak emission bands in the 200-470 nm range related to Y_Al antisite defects and charged oxygen vacancies (F⁺ and F centers). YAG:Ce ОС also possesses significantly larger contribution of slow components in the Ce³⁺ luminescence decay under high-energy excitation in comparison with SC and SCF of this garnet due to the involvement of antisite defects, charged oxygen vacancies as well as boundaries of grains in the energy transfer processes from the host to the Ce³⁺ ions.     

Ce:YAG晶体和透明陶瓷的光学和闪烁性能

采用温梯法生长了Ce:YAG晶体和真空烧结法制备了Ce:YAG透明陶瓷,并对晶体和透明陶瓷的光学和闪烁性能进行了对比研究.Ce:YAG晶体和陶瓷都具有位于230,340和460 nm波段的Ce³⁺离子的特征吸收带和540 nm附近的发射峰,但Ce:YAG晶体同时存在296和370 nm的色心吸收,其发射峰位于398 nm,而透明陶瓷中不存在.Ce:YAG晶体和陶瓷的X射线荧光中均存在520 nm附近的Ce³⁺离子发射,但晶体中还存在由反格位缺陷引起的300 nm 关键词： Ce:YAG 闪烁晶体 透明陶瓷     

Peculiarities of luminescent properties of cerium doped YAG transparent nanoceramics

Optical and luminescence properties of transparent nanosized cerium doped Y₃Al₅O₁₂ (YAG:Ce) ceramics have been studied. YAG:Ce nanoceramics were obtained by means of low temperature and high pressure (LTHP) sintering method. Nanoceramic samples were sintered in the 2–8 GPa pressure range, whereas Ce³⁺ concentration was varied in the 0.5–5 at. % range. It is shown that, in contrast to the single crystal, a strong rise of absorption coefficient was detected already at wavelength shorter than 400 nm in all nanoceramic samples studied. Furthermore, in nanoceramic samples unusual UV emission band near 3.1 eV was observed, which is not observed in the YAG:Ce single crystal. High pressure applied during nanoceramics sintering leads to significant changes in their optical and luminescence properties.     

Scintillation timing characteristics of (La,Gd)2Si2O7:Ce and Gd2SiO5:Ce single crystal scintillators: A comparative study

The scintillation timing characteristics of (La,Gd)₂Si₂O₇:Ce (GPSLa23.5%:Ce) single crystal were studied and compared with Gd₂SiO₅:Ce (GSO:Ce) single crystal. The photoelectron yield, scintillation decay times and coincidence time resolution were measured. At 511 keV γ-rays, the photoelectron yield of 10,770 ± 500 phe MeV⁻¹ and energy resolution of 5.4 ± 0.2% obtained for GPSLa23.5%:Ce are much better than those of 3350 ± 160 phe MeV⁻¹ and 7.8 ± 0.3% obtained for GSO:Ce. The scintillation decay time profile was measured by the time-correlated single photon counting technique using a fast-slow coincidence setup. In both materials the comparable rise times of several nanoseconds are present. The fast component decay time of 56 ns with relative intensity of 49% obtained for GPSLa23.5%:Ce is inferior to that of 32 ns(88%) obtained for GSO:Ce. Consequently, the coincidence time resolution of GPSLa23.5%:Ce is slightly worse than that of GSO:Ce. The normalized time resolution was also discussed in terms of a number of photoelectrons and decay time of the scintillation pulse.     

Luminescence and scintillation properties of Y<Subscript>3</Subscript>A<Subscript>l5</Subscript>O<Subscript>12</Subscript>:Ce single crystals and single-crystal films

Luminescence and scintillation properties of Y₃A_l5O₁₂:Ce single crystals grown from the melt by the Czochralski and horizontal directed crystallization methods in various gas media and Y₃A_l5O₁₂:Ce single-crystal films grown by liquid-phase epitaxy from a melt solution based on a PbO-B₂O₃ flux have been comparatively analyzed. The strong dependence of scintillation properties of Y₃A_l5O₁₂:Ce single crystals on their growth conditions and concentrations of Y_Al antisite defects and vacancy defects has been established. Vacancy defects are involved in Ce³⁺ ion emission excitation as the centers of intrinsic UV luminescence and trapping centers. It has been shown that Y₃A_l5O₁₂:Ce single-crystal films are characterized by faster scintillation decay kinetics than single crystals and a lower content of slow components in Ce³⁺ ion luminescence decay during high-energy excitation due to the absence of Y_Al antisite defects in them and low concentration of vacancy defects. At the same time, the light yield of Y₃A_l5O₁₂:Ce single-crystal films is comparable to that of single crystals grown by directed crystallization due to the quenching effect of the Pb²⁺ ion impurity as a flux component and is slightly lower (∼25%) than the light yield of single crystals grown by the Czochralski method.     

Optical properties and highly efficient laser oscillation of Nd:YAG ceramics

Optical absorption, emission spectra have been measured for polycrystalline Nd-doped Y₃Al₅O₁₂ ceramics. Fluorescence lifetimes of 257.6 μs, 237.6 μs, 184.2 μs and 95.6 μs have been obtained for 0.6%, 1%, 2% and 4% neodymium-doped YAG ceramics, respectively. For the first time, highly efficient laser oscillation at 1064 nm has been obtained with this kind of ceramics. Slope efficiency of 53% has been achieved on a uncoated 4.8-mm thick 1% Nd:YAG ceramics sample. Optical to optical conversion efficiency is 47.6%. Laser oscillation has also been obtained with a 2% Nd:YAG ceramics. The optical properties and laser output results have been compared with that of Nd:YAG single crystal grown by the Czochralski method. Almost identical results have been achieved including laser experiments results. But fabrication of Nd:YAG ceramics is much easier compared to the single-crystal growth method. And also large size (now of about 400 mm diameter×5 mm is available) and high-concentration (>1%) Nd:YAG ceramics can be fabricated. The results show that this kind of Nd:YAG ceramics is a very good alternative to Nd:YAG single crystal. Received: 20 April 2000 / Published online: 16 August 2000     

Timing characteristics of the scintillation response of Gd3Al2Ga3O12:Ce and Gd3Al2.6Ga2.4O12:Ce single crystal scintillators

The timing characteristics of scintillation response of Czochralski-grown Gd₃Al₂Ga₃O₁₂:Ce and Gd₃Al_2.6Ga_2.4O₁₂:Ce single crystals were compared. The photoelectron yield, scintillation decay times, and coincidence time resolution were measured. At 662 keV γ-rays, the photoelectron yield of 6200 phe MeV⁻¹ obtained for Gd₃Al₂Ga₃O₁₂:Ce is higher than that of 4970 phe MeV⁻¹ obtained for Gd₃Al_2.6Ga_2.4O₁₂:Ce, while an inferior energy resolution of the former (7.2% vs. 5.6%) is observed. Scintillation decays are approximated by sum of exponentials with the dominant fast component decay time and its relative intensity of 89 ns (73%) for Gd₃Al₂Ga₃O₁₂:Ce and 136 ns (69%) for Gd₃Al_2.6Ga_2.4O₁₂:Ce. The coincidence time resolution obtained for Gd₃Al₂Ga₃O₁₂:Ce is superior than that of Gd₃Al_2.6Ga_2.4O₁₂:Ce. The normalized time resolution was also discussed in terms of a number of photoelectrons and decay characteristics of the light pulse.     

Luminescence and scintillation characteristics of YAG:Ce single crystalline films and single crystals

The detailed comparative analysis of luminescent and scintillation properties of the single crystalline films (SCF) of YAG:Ce garnet grown from melt-solutions based on the traditional PbO-based and novel BaO-based fluxes, and of a YAG:Ce bulk single crystal grown from the melt by the Czochralski method, was performed in this work. Using the ²⁴¹Am (α-particle, 5.49 MeV) excitation we show that scintillation yield and energy resolution of the optimized YAG:Ce SCF is fully comparable with that of the YAG:Ce single crystal analogue.     

Ce3+-doped crystalline garnet films – scintillation characterization using α-particle excitation

Scintillating properties of Ce³⁺-doped (Lu,Y) aluminum garnet single crystalline films (SCF) were investigated. Thin SCF films of thickness between 1 and 30 μm were grown by a liquid phase epitaxy (LPE) method in various fluxes. The α-particle excitation (mainly 5.4857 MeV line of ²⁴¹Am) of pulse height spectra is used to measure scintillation response of SCF, especially peak of those α-rays which are totally absorbed in the films. Detailed studies and evaluation of scintillation measurements of large sets of Ce³⁺-doped SCF (Lu,Y) aluminum garnets showed that at present time (i) YAG:Ce SCF have comparable scintillation properties as YAG:Ce single crystals, especially their N_phels photoelectron yields are the same while (ii) scintillation properties of LuAG:Ce SCF do not reach those of LuAG:Ce single crystal.     

Single-crystalline films of Ce-doped YAG and LuAG phosphors: advantages over bulk crystals analogues

Luminescent properties of phosphors based on single-crystalline films (SCF) of Y₃Al₅O₁₂:Ce (YAG:Ce) and Lu₃Al₅O₁₂:Ce (LuAG:Ce) garnet have been analyzed in comparison with single-crystal (SC) analogues. It has been shown that the main peculiarity of luminescent properties of YAG:Ce and LuAG:Ce SCF as compared to SC is determined by the extremely low concentration of Y_Al³⁺ and Lu_Al³⁺ antisite defects (AD) in SCF. The advantages of phosphors based on YAG:Ce and LuAG:Ce SCF are caused by the absence in these SCF the additional channels for dissipation of excitation energy connected with AD and vacancy-type defects.     

Potential of GAGG:Ce scintillation crystals for synchrotron X-Ray micro-imaging

We examined the use of cerium-doped gadolinium aluminum gallium garnet (GAGG:Ce) as a material for scintillation screens in synchrotron X-ray radiography (SXR). Highlighted for gamma-ray detection, GAGG:Ce is also an attractive material for SXR because of its high X-ray stopping power and the high light yield at around 530?nm. A thin and transparent screen prepared from our grown ingot of GAGG:Ce was compared with commonly used scintillators of CdWO₄ and YAG:Ce in terms of image quality under monochromatic X-ray illumination. Micron spatial resolutions were achieved with comparable image quality, suggesting that a single crystal of GAGG:Ce is competent scintillation material for SXR.     

Application of LFS-3 crystals as luminescent screens of picosecond image tubes

It is shown that the LFS-3 crystal installed as a luminescent screen in a picosecond image tube provides the shortest afterglow time in comparisonwith all other fast-damping luminescent screens such as Y₃Al₅O₁₂:Ce, Y₂SiO₅:Ce, and others we previously tested under similar conditions. The LFS-3 crystal exposed to single 8-ps pulses of 12–15-keV electrons shows the luminescence decay time no more than 250 ns by the level of 10^-2 of the maximum.     

Light emission efficiency and imaging performance of Y3Al5O12: Ce (YAG: Ce) powder screens under diagnostic radiology conditions

In this study Y₃Al₅O₁₂: Ce powder scintillator was evaluated for use in X-ray imaging detectors. This phosphor, also known as YAG: Ce scintillator or P-46 phosphor, is a non-hygroscopic, emitting green light with very short decay time. These properties are very attractive for X-ray imaging. Y₃Al₅O₁₂: Ce powder was used to prepare various test screens (33–166 mg/cm²). Absolute luminescence efficiency measurements were performed for various X-ray tube voltages (50–130 kVp). In addition parameters related to image quality such as the modulation transfer function and the detective quantum efficiency were examined. A theoretical model, describing radiation and light transfer, was employed to fit experimental data and to estimate values of optical parameters. Absolute efficiency was found to decrease with X-ray tube voltage. Highest efficiency was obtained for the 107 mg/cm² screen. Light attenuation coefficients were close to those of green emitting rare earth scintillators. At low spatial frequencies the detective quantum efficiency was high for the 107–166 mg/cm² screens. The light emission efficiency and imaging performance of Y₃Al₅O₁₂: Ce was not better than currently employed scintillators. However due to its very fast response and high spectral compatibility to optical sensors it may be considered for use in digital imaging detectors.     

Time-resolved luminescent spectroscopy of YAG:Ce single crystal and single crystalline films

The peculiarities of the luminescence and energy transfer from YAG host to the emission centers formed by the Y_Al antisite defects and Ce³⁺ ions have been studied in YAG:Ce single crystals, grown from the melt by modified Bridgman method in Ar and CO₂ + H₂ atmospheres, and YAG:Ce single crystalline film, grown by liquid phase epitaxy method, using the comparative time-resolved luminescent spectroscopy under excitation by synchrotron radiation in the range of fundamental adsorption of this garnet.     

Lu2SiO5:Ce and Y2SiO5:Ce single crystals and single crystalline film scintillators: Comparison of the luminescent and scintillation properties

The paper is dedicated to development of scintillators based on the single crystalline films of Ce³⁺ doped Lu₂SiO₅ (LSO:Ce) and Y₂SiO₅ (YSO:Ce) orthosilicates grown by Liquid Phase Epitaxy method onto YSO substrates from melt-solutions based on the PbO–B₂O₃ flux. We also compare the luminescent and scintillation properties of Ce doped LSO:Ce and YSO:Ce single crystalline films with those of their single crystal counterparts, grown by the Czochralski method.     

Luminescence properties of the Mg co–doped Ce:SrHfO3 ceramics prepared by the Spark Plasma Sintering Method

1300 or 1400 °C pre–sintered Al/Ce/Mg:SrHfO₃ and Al/Ce:SrHfO₃ ceramics were prepared by the Spark Plasma Sintering (SPS) in order to search for a new scintillation material with a high–effective atomic number(Z_eff) and good light output. The SrHfO₃ has a high Z_eff of 60, and high gamma–ray detection efficiency is expected. Meanwhile it has a high melting point of over 2500 °C, and single crystal is hard to be grown. On the other hand, high melting materials can be prepared as ceramics, and the SPS method is a simple process to fabricate the ceramics within a few hours. Thus, we prepared the samples using the SPS method, and their optical and scintillation properties were investigated. We found that Al/Ce/Mg:SrHfO₃ and Al/Ce:SrHfO₃ ceramics had an emission wavelength at around 400 nm originating from 5d–4f transition of Ce³⁺. Moreover, Al/Ce/Mg:SrHfO₃ pre-sintered at a temperature of 1400 °C had a light output of approximately 5,000 ph/MeV. In this paper, the light output of Mg-co-doped samples was improved compared with the Mg-free ones. The light output also depends on the pre-sintering temperature.     

Comparative spectroscopic investigation of Yb3x Y3(1 ? x )Al5O12 (x = 3, 5, 10 and 15%) transparent ceramics

Transparent Yb_3x Y_{3(1 ? x} )Al₅O₁₂ (x = 3, 5, 10 and 15%) ceramics were fabricated by solid-state reaction and vacuum sintering method with a mixture of commercial Al₂O₃, Y₂O₃ and Yb₂O₃ powders. Ethanol and 0.5 wt % tetraethoxysilane were doped. Transparent fully dense samples with grain sizes of several micrometers were obtained by sintered at 1750 K. The absorption spectra, emission spectra and fluorescence life time of these transparent Yb_3x Y_{3(1 ? x} )Al₅O₁₂ ceramics at room temperature have been measured and calculated. The air annealed effects of Yb_3x Y_{3(1 ? x} )Al₅O₁₂ ceramics have been compared with un-annealed Yb:YAG transparent ceramics which shows the difference of the Yb³⁺ ions between annealed and unannealed Yb:YAG ceramics is less than 1%.     

Red, green and blue (RGB) emission doped Y3Al5O12 (YAG) phosphors prepared by non-hydrolytic sol-gel route

An evolutionary optimization process involving combination chemistry was employed in an attempt to develop Y₃Al₅O₁₂ (YAG). The combination chemistry process utilized here consisted the doping of the YAG host with appropriate amounts of red (R), green (G), and blue (B) dopants in a single layer, for use in tricolor white light. The doped YAG was acieved by means of the non-hydrolytic sol-gel route. Four samples were prepared, three of which were mono-doped samples containing 1.0% of a certain lanthanide (Eu³⁺, Tb³⁺, or Tm³⁺) ion, while the fourth contained the three ions. The samples were characterized by X-ray diffractometry and photoluminescence. The diffraction pattern of the mono-doped samples synthered at 800 °C for 16 h displayed peaks corresponding to the Y₃Al₅O₁₂ (YAG) phase, while the sample doped with the three ions revealed the presence of a mixture of Y₃Al₅O₁₂ (YAG) and Y₄Al₂O₉ (YAM) phases. The emission spectra of the three mono-doped YAG samples displayed the typical bands of the blue, green, and red emission of the corresponding lanthanide ions. As for the sample doped with the three lanthanide ions; it simultaneously emitted R, G and B lights. The green emission (546 nm) was more intense and narrow in relation to the red and blue emissions, which may be due to differences in the size of the three incorporated ions.     

Preparation and characterization of transparent Nd:YAG ceramics

Transparent Nd:YAG ceramics were produced by solid.state reaction of high.purity (4N) nanometric oxides powders, i.e., Al₂O₃, Y₂O₃ and Nd₂O₃. After sintering, mean grain sizes of 2% Nd:YAG samples were about 20 μm and their transparency were a bit worse than that of 0.9% Nd:YAG single crystal. Two types of active elements: rods and slabs were fabricated and characterized in several diode pumping schemes. In end pumping configuration as a pump source 20.W fiber coupled laser diode operating in low duty cycle regime (1 ms pump duration/20 Hz) was deployed. In the best case, 3.7 W of output power for 18 W of absorbed pump power, M² < 1.4 were demonstrated for uncoated ceramics Nd:YAG rod of ϕ 4×3mm size in preliminary experiments. For the ceramics of two times lower Nd dopant level above 30% slope efficiency was achieved. In case of Nd:YAG ceramic slab side pumped by 600.W laser diode stack above 12 W was demonstrated with slope efficiency of 3.5%.     

Cr3+:Al2O3透明多晶陶瓷光谱特性分析

对透光性良好的Cr³⁺:Al₂O₃透明多晶陶瓷的光谱性能 进行了研究，其吸收光谱中吸收峰与单晶红宝石相一致，按吸收光谱和Tanabe-Sugano能级 图，算出其晶场强度参数D_q及Racah参数B分别为1792cm^-1， 689cm ^-1，D_q/B=2.6，陶瓷中Cr³⁺离子所处格位的晶体场强 比单晶弱一些，但Cr³⁺:Al₂O₃透明陶瓷仍属于强场晶 体材料；当Cr³⁺掺杂浓度到达0.8wt%时，陶瓷的发射谱仍保持较好的R线发射 ；随Cr³⁺掺杂浓度的增大，激发峰位发生“红移”.在Cr³⁺:Al₂O₃透明多晶陶瓷的荧光谱上，发现一个波长为670nm的发射峰，经激发 谱确认为Cr³⁺的发射峰. 关键词： 氧化铝 透明陶瓷 离子格位 光谱性质