测定古砖年代的光释光和热释光方法的比较研究

采用单片再生剂量光释光法对分布在不同年代(年龄介于180—1600a)的中国古砖样品的等效剂量进行了测定,在测量过程中插入固定的检测剂量来校正样品对光释光的灵敏度变化。同时我们也采用细颗粒常规高温热释光法对砖样的等效剂量进行了测定。这两种方法对照的结果能较好地吻合。得到的等效剂量之比(DeosL/DeTV)介于0．96-1．21之间,平均值为(1．08士0．07)。通过等效剂量和已知年代计算出年剂量为5．07-6．85,与实测的年剂量值相比差别不大。因此,单片再生剂量光释光法用于鉴定古砖样品是一种快速有效的方法。     

Investigation of OSL signals from very deep traps in unfired and fired quartz samples

This paper presents an attempt to isolate experimentally optically stimulated luminescence (OSL) signals which may originate from very deep traps (VDT) in quartz samples. As VDT we consider those traps which are responsible for TL glow peaks with a peak maximum temperature above a TL readout temperature of 500 °C. The basic experimental procedure used to isolate OSL signals from VDT is heating the quartz samples to 500 °C immediately before measuring the OSL signal. The study was carried out on eight quartz samples of very different origins; it is found that all eight samples exhibit OSL signals from VDT, and for a wide region of OSL stimulation temperatures. The OSL signal from VDT depends strongly on the type of quartz sample studied and on whether the sample was fired at high temperatures or not. The behavior of the OSL signal from VDT as a function of the stimulation temperature is found to be very different in fired and unfired samples. The thermal activation energy E for the OSL signals from VDT is obtained in both fired and unfired samples. The OSL signal from VDT in quartz samples fired at 800 °C for 1 h is very high, and the OSL curves consist of three well-defined components and a fourth slow component which is rather poorly resolved. The dose response of these components is obtained using a computerized deconvolution procedure for the dose region 0.5-300 Gy. The results are of importance for dating of ancient fired ceramics, since OSL signals from VDT could potentially extend appreciably the equivalent dose region toward both lower and higher values.     

Investigation of neutron converters for production of optically stimulated luminescence (OSL) neutron dosimeters using Al2O3:C

This paper presents the optically stimulated luminescence (OSL) properties of neutron dosimeters in powder and in the form of pellets prepared with a mixture of Al₂O₃:C and neutron converters. The neutron converters investigated were high density polyethylene (HDPE), lithium fluoride (LiF), lithium fluoride 95% enriched with ⁶Li (⁶LiF), lithium carbonate 95% enriched with ⁶Li (⁶Li₂CO₃), boric acid enriched with 99% of ¹⁰B and gadolinium oxide (Gd₂O₃). The proportion of Al₂O₃:C and neutron converter in the mixture was varied to optimize the total OSL signal and neutron sensitivity. The neutron sensitivity and dose-response were determined for the OSL dosimeters using a bare ²⁵²Cf source and compared to the response of Harshaw TLD-600 and TLD-700 dosimeters (⁶LiF:Mg,Ti and ⁷LiF:Mg,Ti). The results demonstrate the possibility of developing an OSL dosimeter made of Al₂O₃:C powder and neutron converter with a neutron sensitivity (defined as the ratio between the ⁶⁰Co equivalent gamma dose and the reference neutron absorbed dose) and neutron–gamma discrimination comparable to the TLD-600/TLD-700 combination. It was shown that the shape of the OSL decay curves varied with the type of the neutron converter, demonstrating the influence of the energy deposition mechanism and ionization density on the OSL process in Al₂O₃:C.     

A versatile integrated system for thermoluminescence and optically stimulated luminescence measurements

A versatile integrated reader system for TL and OSL measurements of phosphor materials has been described for luminescence research applications. The developed integrated reader system works either in TL or OSL or TL-OSL mode. In the OSL operation, besides the conventional CW-OSL, POSL and LM-OSL modes a novel non-linear OSL (NL-OSL) method has been incorporated in the reader system. The optical stimulation unit consists of four high power LEDs fitted in four channels and optically focused on the sample. Each of the LED is capable of delivering up to 80 mW/cm² light power at the sample position. The LEDs with peak wavelength λ_p ≈ 470 nm and 530 nm and Δλ ≈ 20 nm have been used for optical stimulation of the samples. A PID temperature controller has been used for generating and controlling user defined heating profiles for the TL measurements in the reader system. The reader system covers a wide dynamic dose range of 10 μGy to 10³ Gy for TL/OSL measurements. The OSL grade α-Al₂O₃:C phosphor was used to test the reader system and investigate its impact on low dose assessment for personnel and environmental monitoring. The design concept of the reader system and the results of dose measurements are discussed.     

Simulations of thermally transferred OSL signals in quartz: Accuracy and precision of the protocols for equivalent dose evaluation

Thermally-transferred optically stimulated luminescence (TT-OSL) signals in sedimentary quartz have been the subject of several recent studies, due to the potential shown by these signals to increase the range of luminescence dating by an order of magnitude. Based on these signals, a single aliquot protocol termed the ReSAR protocol has been developed and tested experimentally. This paper presents extensive numerical simulations of this ReSAR protocol. The purpose of the simulations is to investigate several aspects of the ReSAR protocol which are believed to cause difficulties during application of the protocol. Furthermore, several modified versions of the ReSAR protocol are simulated, and their relative accuracy and precision are compared. The simulations are carried out using a recently published kinetic model for quartz, consisting of 11 energy levels. One hundred random variants of the natural samples were generated by keeping the transition probabilities between energy levels fixed, while allowing simultaneous random variations of the concentrations of the 11 energy levels. The relative intrinsic accuracy and precision of the protocols are simulated by calculating the equivalent dose (ED) within the model, for a given natural burial dose of the sample. The complete sequence of steps undertaken in several versions of the dating protocols is simulated. The relative intrinsic precision of these techniques is estimated by fitting Gaussian probability functions to the resulting simulated distribution of ED values. New simulations are presented for commonly used OSL sensitivity tests, consisting of successive cycles of sample irradiation with the same dose, followed by measurements of the sensitivity corrected L/T signals. We investigate several experimental factors which may be affecting both the intrinsic precision and intrinsic accuracy of the ReSAR protocol. The results of the simulation show that the four different published versions of the ReSAR protocol can reproduce accurately the natural doses in the range 0-400 Gy with approximately the same intrinsic precision and accuracy of ∼1-5%. However, these protocols underestimate doses above 400 Gy; possible sources of this underestimation are investigated. Two possible explanations are suggested for the modeled underestimations, possible thermal instability of the TT-OSL traps, and the presence of thermally unstable medium OSL components in the model.     

Precision and accuracy of two luminescence dating techniques for retrospective dosimetry: SAR-OSL and SAR-ITL

Luminescence techniques based on thermally or optically stimulated signals are used extensively for estimating the equivalent dose (ED) of quartz samples for dating and retrospective dosimetry. This paper presents simulations of two luminescence dating protocols which use single aliquots of the quartz samples. The first protocol is the well-known single-aliquot regenerative optically stimulated luminescence (SAR-OSL) protocol for quartz. The second protocol was developed more recently and is based on a thermoluminescence (TL) signal measured under isothermal conditions (termed the SAR-ITL technique). The simulations are carried out using a recently published comprehensive kinetic model for quartz, consisting of 11 electron and hole traps and centers. The complete sequence of the two experimental protocols is simulated using the same set of kinetic parameters. The simulated dose response curves for the two protocols are found to be very similar to published experimental data. The relative intrinsic accuracy and precision of the two techniques is estimated by simulating one hundred random variants of the natural samples, and by calculating the equivalent doses using each technique. The 100 simulated natural variants are generated by keeping the transition probabilities between energy levels fixed, while allowing simultaneous random variations of the concentrations of the 11 energy levels. The SAR-OSL protocol was found to be intrinsically both more accurate and more precise than the SAR-ITL protocol. We investigate several experimental factors which affect the precision and accuracy of the two protocols. New simulations are presented for commonly used sensitivity tests consisting of successive cycles of sample irradiation with the same dose, followed by measurements of the sensitivity corrected L/T signals. These new simulations provide valuable insight into the previously reported sensitivity changes taking place during application of the SAR-ITL protocol.     

Al2O3:C、LiF:Mg,Ti、LiF:Mg,Cu,P对本底辐射的热释光响应比较

用Al2O3:C、LiF:Mg,Ti、LiF:Mg,Cu,P热释光剂量计(TLD)测量湛江市区本底辐射的热释光响应,以选取适合低辐射场辐射剂量测量的TLD。它们的最低响应剂量依次为Al2O3:C(1–2μGy)、LiF:Mg,Cu,P(约2μGy)和LiF:Mg,Ti(>10μGy)。Al2O3:C的热释光峰温较低,对较长时间段(>30 d)的累积剂量,存在较明显的热释光衰退,剂量响应曲线偏离线性;LiF:Mg,Cu,P和LiF:Mg,Ti的发光峰温较高,数年内都很稳定。综合考虑灵敏度和稳定性,LiF:Mg,Cu,P更宜于低辐射场的累积剂量测量。     

Thermoluminescence properties of nanocrystalline K2Ca2(SO4)3:Eu irradiated with gamma rays and proton beam

Thermoluminescence properties of nanocrystalline K₂Ca₂(SO₄)₃:Eu prepared by ball milling technique have been studied and the nanophosphor’s suitability as an effective gamma radiation and proton beam dosimeter material has been examined. It is found that the nanophosphor is suitable for dosimetry over a very wide range of doses ∼1 Gy to 1 kGy for gamma radiation. And for proton beam the same nanophosphor shows a more or less linear response for the dose range 0.1-100 Gy. A comparative study of this nanophosphor with its corresponding microcrystalline form (prepared by solid-state diffusion method) as well as the nanocrystalline form prepared by (the more conventional) co-precipitation technique has shown that the nanophosphor prepared by the ball milling technique is in almost all respects better than the other two forms reported earlier.     

粉末Ba0.95M0.05FBr：Eu^2＋（M=Sr,Ca）的光激励发光研究

BaFBr:Eu^2 、Ba0.95Sr0.05FBr:Eu^2 以及Ba0.95Ca0.05FBr:Eu^2 粉末样品中在未经X射线或紫外光辐照之前,用长波长（＞400nm）光激励样品。都可观测到对应于Eu^2 4f^65d→4f^7跃迁的390nm发光,发光与样品制备过程中形成的F心有关。在样品的激励光谱中可以观测到两组峰,中心峰值于535nm的峰相应于F（F^- )心电子的激励,而峰值位于708nm的峰可能源于F(Br^-）心或F(Br^-）心聚合体电子的激励。当少量（5％）半径较小的碱士金属离子Ca^2 （半径为0．0099nm）或Sr^2 （半径为0．113nm）替代Ba^2 （半径为0．135nm）进入晶格时,随着离子半径的减小,位于535nm和708nm的激励峰强度随这减小,而且分别在580nm和650nm或575nm和645nm处出现肩峰,在波长为50－400nm的吸收光谱中减小,而且分别在580nm和650nm或575nm和645nm处出现肩峰,在波长为50－400nm的吸收光谱中发现,由于小半径碱士金属离子的替代,79nm和83nm吸收峰红移,且出现新的吸收峰。证实了Sr^2 或Ca^2 部分替代Ba^2而产生新生的替代Ba^2 而产生新的色心：F（F^-,Sr^2 )、F(Br^-,Sr^2 ）心或F(F^－,Ca^2 )、F(Br^-,Ca^2 )心,也应于激励光谱中出现的肩峰。     

A XAS study of the local environments of cations in (U, Ce)O2

Mixed oxide (MOX) fuel is usually considered as a solid solution formed by uranium and plutonium dioxides. Nevertheless, some physico-chemical properties of (U_1−y, Pu_y)O₂ samples manufactured under industrial conditions showed anomalies in the domain of plutonium contents ranging between 3 and 15 at.%. Cerium is commonly used as an inactive analogue of plutonium in preliminary studies on MOX fuels. Extended X-ray Absorption Fine Structure (EXAFS) measurements performed at the European Synchrotron Radiation Facility (ESRF) at the cerium and uranium edges on (U_1−y, Ce_y)O₂ samples are presented and discussed. They confirmed on an atomic scale the formation of an ideal solid solution for cerium concentrations ranging between 0 and 50 at.%.     

Glass-ceramic nuclear waste forms obtained from SiO2-Al2O3-CaO-ZrO2-TiO2 glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): study of internal crystallization

Glass-ceramic waste forms such as zirconolite (nominally CaZrTi₂O₇) based ones can be envisaged as good candidates for minor actinides or Pu immobilization. Such materials, in which the actinides (or lanthanides used as actinide surrogates) would be preferentially incorporated into zirconolite crystals homogeneously dispersed in a durable glassy matrix, can be prepared by controlled crystallization (nucleation + crystal growth) of parent glasses belonging to the SiO₂-Al₂O₃-CaO-ZrO₂-TiO₂ system. In this work we present the effects of the nature of the minor actinide surrogate (Ce, Nd, Eu, Gd, Yb, Th) on the structure, the microstructure and the composition of the zirconolite crystals formed in the bulk of the glass-ceramics. The amount of lanthanides and thorium incorporated into zirconolite crystals is discussed in relation with the capacity of the glass to accommodate these elements and of the crystals to incorporate them in the calcium and zirconium sites of their structure.     

A track structure model of optically stimulated luminescence from Al2O3:C irradiated with 10-60 MeV protons

We investigated the optically stimulated luminescence (OSL) signal from Al₂O₃:C irradiated with 10-60 MeV protons to estimate the potential use of this material as a proton dosimeter. After irradiation, OSL decay curves were read out and we used both the initial part and the total area of these curves as response signal. A precondition for optimal proton dosimetry is an LET-independent response and the experimental data showed such an independence at 0.3 Gy for the initial OSL signal.To understand the experimental results, we applied target and track structure theory. Here, the OSL signal is considered to be a result of target activation and the OSL proton signal is calculated from the OSL gamma signal and a radial dose distribution around the proton track. Although several simplifications were made to ease calculations, the classic track structure theory can qualitatively account for all the main features of the experimental data. We estimate a target radius to be between 30 and 150 nm and associate this radius with a charge migration distance in the crystal.The model calculations suggest that the dose and LET-dependency of the OSL signal is a result of an unique mixture of one- and two-hit targets. This implies that the initial OSL signal from Al₂O₃:C in general is not LET-independent at 0.3 Gy or lower doses. However, a mixture of the initial and total OSL signal could provide an LET-independent response in a given LET and dose interval.     

Blue luminescence from poly(methyl methacrylate) modified ZnO and anatase TiO2 nanocrystals prepared using γ radiation

The surface of ZnO and anatase TiO₂ nanocrystals was modified by PMMA through γ radiation. The modified nanocrystals were investigated with photoluminescence (PL) and Fourier transform infrared (FTIR) spectra. A stable blue luminescence peak (420 nm) can be observed for the modified ZnO and anatase TiO₂ nanocrystals. The intensities of luminescence of the modified ZnO and anatase TiO₂ in aqueous solution are very stable, even unchanged after storage time of one month.     

一种潜在5-HT1A脑受体显像剂99Tcm-Bicine/HYNIC-MPP2的制备及其生物性能

优化合成了含有1-(2-甲氧基苯基)哌嗪(MPP)结构的配体2-(4-(2-甲氧基苯基)哌嗪基)乙胺-6-叔丁基氧羰基肼基吡啶-3-甲酸(HYNIC-MPP2).在室温下以N,N-二(2-羟基乙基)氨基乙酸(Bicine)为共配体制备得到配合物~(99)Tc~m-Bicine/HYNIC-MPP2,其放射化学纯度大于95%,并且在6 h内保持稳定.脂水分配系数和电泳实验结果表明,该放射性标记配合物是水溶性和电中性的.正常小鼠体内生物分布实验结果表明,~(99)Tc~m-Bicine/HYNIC-MPP2有一定的脑摄取(注射后2 min时为0.31%ID/g).脑区域分布及抑制实验显示,该配合物在5-HT_(1A)受体含量丰富的海马组织有较高摄取(注射后2 min时为1.00%ID/g),而在受体含量低的小脑组织中摄取也低(注射后2 min时为0.63%ID/g).抑制后,海马摄取降低较多(注射后2 min时为0.42%ID/g),而小脑摄取则无明显变化.抑制前后海马/小脑比值分别为1.59和0.89.由此可见该标记配合物与5-HT_(1A)受体具有一定特异性结合,是一种新的潜在5-HT_(1A)受体显像剂.     

肿瘤PET分子探针3-O-(2-18F-氟乙基)-L-多巴的合成及初步生物学评价

正电子类氨基酸显像剂是¹⁸F-氟代脱氧葡萄糖（¹⁸F-Fluorodeoxyglucose,¹⁸F-FDG）在临床肿瘤PET显像应用中的重要补充。针对6-¹⁸F-氟-L-多巴（¹⁸F-FDOPA）前体制备及标记过程的复杂性,本研究设计合成了一种新型¹⁸F-标记的氨基酸类肿瘤PET显像剂3-O-(2-¹⁸F-氟乙基)-L-多巴（3-O-(2-¹⁸F-fluoroethyl-L-DOPA,¹⁸F-FEDOPA）,并对其内生物分布及肿瘤PET显像进行了评价。以L-多巴（L-DOPA）为原料经多步反应合成标记前体化合物-N-叔丁氧羰基-(3-O-甲苯磺酸酯乙基-4-O-叔丁氧羰基)-L-多巴甲酯,通过¹⁸F-亲核取代反应实现放射性标记,经半制备高效液相色谱纯化、盐酸水解、NaOH中和后得到¹⁸F-FEDOPA注射液。放化合成时间为90 min,放化产率（33±6）%（n=10,衰减校正）,放射性比活度为55 GBq/μmol,放化纯度>99％,4 h后测定放化纯度>95%,稳定性良好。小鼠体内生物分布表明,¹⁸F-FEDOPA主要经肾脏代谢,心脏和脑组织摄取值较低,骨骼摄取随时间无明显变化。microPET/CT显像显示,¹⁸F-FEDOPA在H22和S180肿瘤组织有明显摄取;与¹⁸F-FDG相比,¹⁸F-FEDOPA在注射60 min时肿瘤与心（或脑）的比值高。因此,¹⁸F-FEDOPA有望成为一种新型氨基酸代谢类肿瘤PET显像剂。     

Film growth by polyatomic C2H5 bombarding a diamond (1 0 0) surfaces: Molecular dynamics study

The deposition of polyatomic C₂H₅⁺ ions is studied using classical molecular dynamics simulations with a new improved Brenner potentials developed by Brenner. The simulation results show that when the incident energy is less than 65 eV, the deposition coefficient of H is larger than that of C atoms. When the incident energy is larger than 65 eV, the deposition of H is less than that of C atoms. With increasing incident energy, a transition from Csp3-rich to Csp2-rich in the grown films is found.     

Resonant ion stimulated desorption of O from the TiO2(1 1 0) surface: Effects of oxygenation and ion bombardment

The O⁺ desorption from reduced, oxygenated, and ion-bombarded TiO₂(1 1 0) surfaces has been investigated during He⁺ irradiation. The O⁺ desorption is initiated by creation of an antibonding O 2s core hole state via quasi-resonant charge exchange with the He⁺ 1s state, followed by the intra-atomic Auger decay of the O 2s hole. Upon oxygenation of the reduced TiO₂(1 1 0) surface, the O⁺ yield increases by one order of magnitude. The O₂ molecule is dissociated at the vacancy site of bridging oxygen and the oxygen atoms either fill a vacancy site or chemisorb at a fivefold-coordinated Ti⁴⁺ site as an adatom. The latter is detected with much higher efficiency than the former. The O⁺ yield is increased during He⁺ bombardment of the reduced TiO₂(1 1 0) surface due to formation of lower coordinated oxygen atoms. The oxygen species thus formed by ion bombardment or oxygenation are unstable on the surface and tend to diffuse into bulk vacancy sites or higher coordination surface sites even at room temperature.