Optically stimulated luminescence: Searching for new dosimetric materials

Optically stimulated luminescence (OSL) is increasingly being used as a dosimetric technique in various fields such as medical, environmental and space dosimetry, and sediment and archaeological dating. Nevertheless few compounds are suitable as OSL materials. In this work, a survey was made of various insulators, searching for candidates for new OSL dosimeters. Natural and synthetic crystals and glasses from numerous sources are included. Luminescence was stimulated with blue LEDs (470 nm) and with IR laser (830 nm) provided by an automatic reader. Irradiation was performed with a ⁹⁰Sr/⁹⁰Y beta source, and the emitted light was measured with a photomultiplier tube, protected with suitable optical filters. Thermoluminescence (TL) of the samples was also measured, with the same equipment, to evaluate the thermal and optical stability of the defects related to OSL and TL. Among the various investigated materials, Al₂O₃:Cr, Mg, Fe, MgAl₂O₄ spinels, Mg₂SiO₄:Tb, and natural fluorite show potential as OSL dosimeters. Some materials, as barium aluminoborate glasses, although showing intense OSL signals, present a high fading at room temperature. In that situation the OSL signal is related to low temperature TL peaks that also fade at room temperature. None of the investigated materials was specially prepared to be used as an OSL dosimeter, which means that work can be done, mainly in the impurity nature and content, in order to improve OSL signals and to overcome some of the shortcomings that were noticed.     

Heavy ion irradiation effects in the rare-earth sesquioxide Dy2O3

Polycrystalline pellets of the rare-earth sesquioxide Dy₂O₃ with cubic C-type rare-earth structure were irradiated with 300 keV Kr²⁺ ions at fluences up to 5 × 10²⁰ Kr/m² at cryogenic temperature. Irradiation-induced microstructural evolution is characterized using grazing incidence X-ray diffraction (GIXRD) and transmission electron microscopy (TEM). In previous work, we found a phase transformation from a cubic, C-type to a monoclinic, B-type (C2/m) rare-earth structure in Dy₂O₃ during Kr²⁺ ion irradiation at a fluence of less than 1 × 10²⁰ Kr/m². In this study, we find that the crystal structure of the top and middle regions of the implanted layer transform to a hexagonal, H-type (P6₃/mmc) rare-earth structure when the irradiation fluence is increased to 5 × 10²⁰ Kr/m²; the bottom of the implanted layer, on the other hand, remains in a monoclinic phase. The irradiation dose dependence of the C-to-B-to-H phase transformation observed in Dy₂O₃ appears to be closely related to the temperature and pressure dependence of the phases observed in the phase diagram. These transformations are also accompanied by a decrease in molecular volume (or density increase) of approximately 9% and 8%, respectively, which is an unusual radiation damage behavior.     

Neutron beam design for both medical neutron capture therapy and industrial neutron radiography for TRIGA reactor

Neutron beam designs were studied for TRIGA reactor with a view to generating thermal, epithermal and fast neutron beams for both medical neutron capture therapy (NCT) and industrial neutron radiography (NR). The beams are delivered from thermal and thermalizing columns, and also horizontal beam hole. Several prospective neutron filters (high-density graphite (G), bismuth (Bi), single-crystal silicon (Si), aluminum (Al), aluminum oxide (Al₂O₃), aluminum fluoride (AlF₃) and lead fluoride (PbF₂)) were examined for obtaining sufficiently intense neutron beam for various applications. Monte Carlo calculations indicated that with a suitable neutron filter arrangement, thermal and epithermal neutron beams attaining 2×10⁹ and 7×10⁸ n cm⁻²S⁻¹, respectively, could be obtainable from thermal and thermalizing columns with the reactor operating at 100 kW. These neutron beams could be adopted for boron neutron capture therapy. Compared with these columns, horizontal beam port would deliver neutron fluxes of 10⁻² 10⁻³ lower intensity, but produced thermal and neutron beams would be adequate for different application of nondestructive inspection by neutron radiography.     

应用可调谐外腔半导体激光器测量锂同位素比率

采用中心波长固定的可调谐外腔半导体激光器作为光源,通过激光吸收光谱法对锂原子同位素比率进行测量。该方法利用PID温控器实现锂金属蒸发温度的控制和测量。采用激光斜入射的方式消除光路调试过程中产生的标准具效应。实验测量给出了6组不同腔体温度下⁶Li和⁷Li在671 nm附近的吸收光谱,通过对⁶LiD₁和⁷LiD₂吸收峰进行积分吸收计算,得到⁶Li/⁷Li同位素比率测量精度可达2.5%。     

离子液体/苯并15-冠-5浸渍XAD-7树脂萃取分离锂同位素

以XAD-7树脂为支撑担体制备了含有三种不同咪唑型离子液体([C_8mim][BF_4]、[C_8mim][PF_6]、[C_8mim][(SO_2CF_3)_2N])和萃取剂(苯并15-冠-5)的浸渍树脂,并用于锂同位素的萃取分离。浸渍树脂的红外和扫描电镜表征表明,离子液体成功负载到了树脂上;热重分析表明,该浸渍树脂具有良好的热稳定性。在水相初始pH=5.55时,浸渍树脂具有最佳萃取率。浸渍树脂在LiSCN溶液中具有较高的萃取率,而在CF_3COOLi溶液中呈现较大的单级分离因子,最大单级分离因子达到1.045±0.002。浸渍树脂的萃取平衡时间为2.5~3h。萃取热力学研究表明,该反应为自发过程,温度对体系的影响较小。~6Li富集于固相,~7Li富集在水相。该系列浸渍树脂易于再生,可循环使用。     

Time Dependent DD Neutrons Measurement Using a Single Crystal Chemical Vapor Deposition Diamond Detector on EAST

A single crystal chemical vapor deposition(scCVD) diamond detector has been successfully employed for neutron measurements in the EAST(Experimental Advanced Superconducting Tokamak) plasmas.The scCVD diamond detector coated with a 5 μm ~6LiF(95%~6Li enriched) layer was placed inside a polyethylene moderator to enhance the detection efficiency.The time-dependent neutron emission from deuteron plasmas during neutral beam injection(NBI)heating was obtained.The measured results are compared with that of fission chamber detectors,which always act as standard neutron flux monitors.The scCVD diamond detector exhibits good reliability,stability and the capability to withstand harsh radiation environments despite its low detection efficiency due to the small active volume.     

基于铌酸银的耐高温放射性碘吸附剂的制备及性能

通过机械混合法制备了一种基于铌酸银(AgNbO_3)的耐高温放射性碘吸附剂(AgNbO_3/Al_2O_3)。和常规载银吸附剂(Ag/Al_2O_3)相比,AgNbO_3/Al_2O_3吸附剂的吸附性能更为稳定;特别是在650℃以上时,其对放射性碘的去污因子远高于常规载银吸附剂。表征测试结果表明,该吸附剂结构稳定性良好,可耐受较长时间的高温。热重测试和高温脱附试验等结果表明,碘化银在AgNbO_3/Al_2O_3吸附剂表面稳定性的提高是该吸附剂在高温时吸附性能更佳的主要原因,其将来有望用于核事故中的应急处置。     

UiO-66-(COOH)2的合成及其对锂同位素吸附分离性能研究

为研究金属有机骨架材料对⁷Li的吸附分离性能,本研以水作为溶剂,四氯化锆和均苯四甲酸为起始原料,采用水热法合成金属有机骨架材料UiO-66-(COOH)₂,对合成材料的形貌、孔径、热稳定性等进行表征与分析;通过静态吸附实验探讨吸附时间、反应温度、溶液浓度对UiO-66-(COOH)₂锂离子吸附性能及同位素分离因子的影响;并对Li⁺浓度、⁶Li/⁷Li同位素丰度进行测定。结果表明,UiO-66-(COOH)₂可实现对锂的吸附以及⁷Li的分离,且在293 K Li₂CO₃溶液中,每0.05 g UiO-66-(COOH)₂对10 mL 0.05 mol/L Li₂CO₃进行4 h的静态吸附,最大吸附量Q为9.53 mg/g,分离因子S（⁷Li/⁶Li）为1.019 54。研究结果为⁷Li的分离提供了新途径。     

Na_2O/Al_2O_3摩尔比对模拟高放废液硼硅酸盐玻璃固化体结构和性能的影响

研究了Na2O/Al2O3摩尔比(n)对模拟高放废液硼硅酸盐玻璃固化体结构和性能的影响。利用红外光谱分析了不同Na2O/Al2O3摩尔比时硼硅酸盐玻璃固化体的结构变化,并用溶解速率法(DR)和全谱直读等离子发射光谱(ICP-OES)表征了所制备出固化体的化学稳定性。结果表明:在研究组分范围内,当n1.0时,硼硅酸盐玻璃固化体结构中Al以[AlO4]四面体的形式存在,但[BO3]三角体的量较大;随着Na2O/Al2O3摩尔比的增加(n=1.0),固化体结构中[BO3]三角体向[BO4]四面体转变,Al仍以[AlO4]四面体的形式存在,固化体结构稳定性增加;Na2O/Al2O3摩尔比继续增加(n=1.5或2.0),固化体成分中由于Al含量已很少而使[AlO4]含量过少,对固化体结构网络致密性的影响起主要作用,且此时成分中存在过多的碱金属离子在结构中起断网作用,玻璃固化体网络结构变疏松。在Na2O/Al2O3摩尔比为1.0时,玻璃固化体有相对较佳的结构稳定性和化学稳定性,浸泡56d后的失重速率为10-9 g/(cm2·min)数量级,且浸出液中各浸出离子的平均浓度最低。     

Post-irradiation examination of uranium-doped rock-like oxide fuels

Post-irradiation examinations of rock-like oxide fuels were performed in JAERI to evaluate irradiation behavior and geochemical stability. Five kinds of fuels were prepared using 20% enriched U instead of Pu; a single-phase fuel of an yttria-stabilized zirconia containing UO₂ (U-YSZ), two particle-dispersed type fuels of U-YSZ particles + MgAl₂O₄/Al₂O₃ powder, two homogeneously blended type fuels of U-YSZ powder + MgAl₂O₄/Al₂O₃ powder. The fuels were irradiated in JRR-3 for about 100 days and estimated irradiation conditions were as follows; linear power was 15 kW m⁻¹, thermal neutron fluence was 7 x 10²⁴ m⁻² and fuel temperatures at the surface were 740–1130 K. From the results of non-destructive examinations, the stainless steel cladding surfaces were partially discolored by oxidation and no remarkable deformation of the pins was observed. Significant pellet fragmentation was not observed in spite of the crack formation as observed in irradiated LWR UO₂ fuels. Nonvolatile FPs were observed only in pellets but volatile Cs moved partly to the plenum. From these examinations, no significant difference in macroscopic irradiation behavior was distinguished among 5 fuels.     

keV能区中子注量率测量初级标准装置研制

由于大多数中子探测器在keV能区处于共振能区,截面数据无法精确已知,无法作为中子注量率测量初级标准装置。⁶Li在keV能区的截面精确已知,本文以此设计了一种包含⁶LiF转换体的硅半导体探测器系统（LiF-SSD探测器）,建立了keV能区中子参考辐射场中子注量率测量初级标准装置。利用SRIM和TRIM程序估算了LiF-SSD探测器的计数率;基于Geant4开发了探测器响应计算程序,给出了中子能量为27.4 keV的探测器脉冲幅度计算谱;利用⁴⁵Sc(p,n)-⁴⁵Ti反应,测量了27.4 keV中子能量点的探测器脉冲幅度谱,测量结果与理论计算谱符合较好。     

α/γ相比率调控对超音速等离子喷涂Al2O3阻氚涂层微结构及性能的影响

采用超音速等离子喷涂技术在中国低活化马氏体钢表面制备不同α/γ相比率的Al₂O₃阻氚涂层,研究了α/γ相比率调控对Al₂O₃涂层微观结构、力学性能和耐电化学腐蚀性能的影响。利用掠入射X射线衍射（GIXRD）和扫描电子显微镜（SEM）表征Al₂O₃涂层的微观结构、粘结拉伸试验法和纳米压痕仪表征涂层的力学性能、动电位极化曲线法测试涂层的耐电化学腐蚀性能。研究结果显示：通过调控特征喷涂参数（CPSP）,Al₂O₃涂层中α相含量从78.6%至24.4%可控调节,且孔隙率从2.8%降低至1.5%;α相含量为78.6%的Al₂O₃涂层硬度为(11.500±0.575) GPa,约为高γ相含量(75.6%)涂层的2倍;且高α相含量(78.6%)涂层的腐蚀电流密度较高γ相含量(75.6%)涂层的腐蚀电流密度低1个数量级。以上结果表明,高α相含量(78.6%)的Al₂O₃涂层具有更优异的力学性能、耐电化学腐蚀性能以及耐Cl^-扩散穿透能力,具有应用于聚变堆结构材料表面阻氚涂层的潜能。     

Post irradiation examination of uranium inclusions in inert matrices.

The inert matrix materials CeO₂, MgO, Y₂O₃, MgAl₂O₄ and Y₃Al₅O₁₂ were selected as candidates for inert matrices for the EFTTRA²-T3 neutron irradiation experiment. Most targets contain 20% enriched ²³⁵U fissile inclusions with an average size of roughly 150 μm. The volume fraction of the fissile phase is either 2.5 vol% UO₂ or 19.6 vol% of Y_5.78UO_x in the inert matrices. The samples were irradiated for 198.9 full power days in the High Flux Reactor in Petten. The calculated burn-up is between 17.3 and 19.5% FIMA. The temperature of the cladding was kept at 600 ± 25 K. A dimensional change of at least +5 % is measured after neutron irradiation for Y₃Al₅O₁₂ and MgAl₂O₄ with macro dispersions of UO₂; the other targets with a macro dispersion of UO₂ show a volume change of less than + 1 vol%. The fractional release of the fission gas Xe is more than 40% for the MgAl₂O₄ and Y₃Al₅O₁₂ matrices with a macro dispersion of UO₂, the other targets show a fractional release of Xe of less than 15%. Cracks are observed in MgO and MgAl₂O₄ targets which is possibly related to the stress caused by swelling of the UO₂ inclusions.     

Low-temperature diffusion in inert-gas bombarded Al2O3

Previous work on diffusion in inert-gas bombarded Al₂O₃ has revealed the presence of four diffusion processes, of which two take place well below the temperatures for self-diffussion, one agrees with self-diffusion, and one occurs at temperatures well above those for self-diffusion. The present work serves to explore in greater detail the two low-temperature processes. It is shown that the first, which is found in -Al₂O₃, Al(OH)₃, and γ-Al₂O₃beginning at about 100° C, is consistent with a range of ΔH's of 28 to 50 kcal/mole. The mechanism of the process is hinted at by the fact that it overlaps the temperatures both for Al(OH)₃decomposition and for point-defect motion in -Al₂O₃; the correlation with point defects is believed, however, to be the more significant. The second process, which is found only in -Al₂O₃ beginning at 500–650° C, implies an essentially single ΔH lying between 69 and 79 kcal/mole. It was suggested previously by Matzke and Whitton on the basis of electron diffraction that the process could be attributed to the amorphous-crystalline transition of -Al₂O₃. Further aspects of low-temperature diffusion in Al₂O₃ were revealed by comparing autoradiographs of specimens of -A₂O₃which were bombarded to various doses and then either heated to 850° C or immersed in unheated 12N NaOH. Thus regions exposed to a high dose and which would be expected to be amorphous, had an increased sticking factor, a greater tendency to lose gas during heating, and an enhanced chemical reactivity.     

Mo在Al2O3上的吸附、解吸性能及其与U、Sr、Cs、I等杂质元素的分离

目前国际⁹⁹Mo面临供应危机,急需新技术和新反应堆。医用同位素生产堆是以²³⁵UO₂(NO₃)₂溶液为燃料的专用反应堆,生产成本低、三废少、经济效益高。本工作利用Al₂O₃为分离材料,从模拟的医用同位素生产堆（MIPR）燃料溶液中分离和纯化Mo。结果表明,经两次分离,Mo的总回收率大于 60%, U、Sr、Cs、I等杂质可以被除去,采用Al₂O₃从MIPR燃料溶液中提取⁹⁹Mo工艺可行。     

Argon irradiation damage at a Cu/Al2O3 interface for different alumina structures

The evolution of damages at a Cu/Al₂O₃ device interface after Ar⁺ irradiation, depending on alumina structure, and the effect of surface roughness on sputtering have been studied. A polycrystalline Cu/Al₂O₃ bilayer and polycrystalline Cu on amorphous alumina were irradiated with 400 keV Ar⁺ ion beam at doses ranging from 5 × 10¹⁶ to 10¹⁷ Ar⁺/cm² at room temperature. The copper layer thicknesses were between 100 and 200 nm. RBS analysis was used to characterize the interface modification and to deduce the sputtering yield of copper. The SEM technique was used to control the surface topography. A RBS computer simulation program was used to reproduce experimental spectra and to follow the concentration profile evolutions of different elements before and after ion irradiation. A modified TRIM calculation program which takes into account the sputtering yield evolution as well as the concentration variation versus dose gives a satisfactory reproduction of the experimental argon distribution. The surface roughness effect on sputtering and the alumina structure influence at the interface on mixing mechanisms are discussed.     

用于快中子能谱测量的6LiF夹心半导体谱仪

本文介绍了^{6LiF夹心谱仪的测量原理、自行设计研制的6LiF夹心半导体谱仪探头结构及电子学系统组成等。在热中子场中测试了夹心谱仪的性能,获得了α粒子峰、T粒子峰及“和”峰在多道上的位置与能量分辨率,并用T粒子与“和”峰两个能量点的峰位对谱仪系统进行了能量刻度。分别用效应探头和本底探头测量了临界装置表面的效应谱和本底谱,当效应探头采用的6LiF镀层质量厚度为186 μg/cm2时,6LiF夹心谱仪对热中子的能量分辨率为363 keV,测量中子最佳能区为0.3~7.5 MeV,在该能区内,本底谱约占1%。}     

Investigation of Stable Al2O3 Scale on Fe-Al Aluminized Coating for Tritium Barrier

It is well known that α-Al₂O₃ phase has stablility performance, high permeation reduction factor and good resistance performance in liquid LiPb, which is considered as the reference tritium barrier coating in future fusion reactor. In order to study the formation mechanism of stable α-Al₂O₃ scales on fusion structure material, the oxidation behavior of Fe-Al aluminized coating on China Low Activated Martensitic （CLAM） steel was investigated under the oxygen partial pressure from 1 Pa to 20 kPa at the temperature of 940-980 ℃. The Al₂O₃ scales were analyzed by thermogravimetric analysis meter, grazing angle X-ray diffractometer, glow discharge spectrometer, focused ion beam and transmission electron microscope. A single continuous Al₂O₃ scales with the maximum thickness of about 2 000 nm was formed on the diffusion Fe-Al aluminized layer. Thermogravimetric analysis results show that the higher oxidation rate constant is achieved while increasing the oxygen partial pressure, and then oxidation rate constant decreases. The phase transformation of Al₂O₃ scales on the surface of Fe-Al aluminized coating was studied during different oxidation time ranges from 3 min to 180 min. The metastable γ-Al₂O₃ and α-（Al0.948Cr0.052）₂O₃ phases is formed in the earlier oxidation process and finally transformed to stable α-Al₂O₃ phase. The features of the transient α-（Al0.948Cr0.052）₂O₃（113） and α-Al₂O₃（113） were detected by GXRD and then confirmed by focused ion beam and transmission electron microscope.     

Melting behaviour of oxide systems for heterogeneous transmutation of actinides. II. The system MgO–Al2O3–PuO2

Isothermal sections of the phase diagram of the system MgO–Al₂O₃–PuO₂ at various temperatures were calculated using sublattice models. The results show that below 2133 K no liquid occurs in the system. Above 2133 K liquid starts to form at the Al₂O₃–PuO₂ side. The phase diagram of the pseudo-binary system PuO₂–MgAl₂O₄ was also obtained from an isopleth T–x calculation.     

Transformation of Al2O3 to LiAlO2 in Pb–17Li at 800 °C

A FeCrAl substrate was pre-oxidized for 2 h at 1000 °C to thermally grow an external Al₂O₃ scale and then isothermally exposed to Pb–17 at.% Li for 1000 h at 800 °C to determine if this layer would protect the underlying alloy from dissolution. After exposure, a small mass gain was measured, indicating that the layer did inhibit dissolution. However, characterization of the external layer determined that it had transformed to LiAlO₂ with an increased thickness and a much larger grain size than the original layer. This observation has implications for the use of Al₂O₃ as a permeation barrier in Pb–Li cooled fusion blanket systems.