Effect of high-dose irradiation on the optically stimulated luminescence of Al2O3:C

This paper examines the effect of high-dose irradiation on the optically stimulated luminescence (OSL) of Al2O3:C, principally on the shape of the OSL decay curve and on the OSL sensitivity. The effect of the degree of deep trap filling on the OSL was also studied by monitoring the sensitivity changes after doses of beta irradiation and after step-annealing of samples previously irradiated with high doses. The OSL response to dose shows a linear-supralinear-saturation behavior, with a decrease in the response for doses higher than those required for saturation. This behavior correlates with the sensitivity changes observed in the samples annealed only to 773 K, which show sensitization for doses up to 20-50 Gy and desensitization for higher doses. Data from the step-annealing study leads to the suggestion that the sensitization is caused by the filling of deep electron traps, which become thermally unstable at 1100-1200 K, whereas the desensitization is caused by the filling of deep hole traps, which become thermally unstable at 800-875 K, along with a concomitant decrease in the concentration of recombination centers (F+ -centers). Changes in the shape of the OSL decay curves are also observed at high doses, the decay becoming faster as the dose increases. These changes in the OSL decay curves are discussed in terms of multiple overlapping components, each characterized by different photoionization cross-sections. However, using numerical solutions of the rate equations for a simple model consisting of a main trap and a recombination center, it is shown that the kinetics of OSL process may also be partially responsible for the changes in the OSL curves at high doses in Al2O3:C. Finally, the implication of these results for the dosimetry of heavy charged particles is discussed.     

Intrinsic superlinear dose dependence of thermoluminescence and optically stimulated luminescence at high excitation dose rates

Superlinear dose dependence of thermoluminescence (TL) and optically stimulated luminescence (OSL) has been reported for many materials. The theoretical explanation has been ascribed to competition of either traps or recombination centers, during the excitation stage or during the read-out phase. There has been an account in the literature on superlinearity of OSL associated with merely one trapping state and one kind of recombination center. This had to do with the process taking place during the read-out stage, namely the optical stimulation. In the present work, we report on a model of one trapping state and one kind of recombination center which results in a superlinear filling of the center. Thus, one can expect a superlinear dose dependence of the area under the resulting TL glow peak as well as the OSL signal. We follow this situation by writing the simultaneous nonlinear rate equations for the one-trap-one-recombination-center (OTOR) model and study the expected results by numerical simulation consisting of solving the equations with sets of the trapping parameters. We also present analytical results based on simplifying assumptions, and compare the analytical and numerical results. The effect is significant at relatively high dose rates. The main implication is that when one tries to evaluate by TL dosimetry a dose applied at a high rate, calibration of the TL dosimeter using much smaller dose rates may result in inaccurate results.     

Optically stimulated luminescence (OSL) study of synthetic stishovite

Optically stimulated luminescence (OSL) of synthetic stishovite was investigated for a future dating technique of meteor impact craters. Luminescence around 330 nm was measured on the γ-ray irradiated stishovite under two stimulating light sources of infrared laser (830 nm) and blue light emitting diode set (470 nm). Thermoluminescence (TL) studies before and after the OSL measurements showed the intensities around 100–200°C and 220–350°C to increase and those around 350–450°C to decrease. This indicates that a part of deep-trapped charges excited during the OSL measurements were retrapped by shallower traps. The infrared stimulated luminescence (IRSL) after the TL measurement up to 450°C could not be detected, while the blue light stimulated luminescence (BLSL) after TL had about one-tenth of the intensity before TL. This indicates that a part of the charges in shallower traps were detrapped thermally and returned to the deeper traps which were related to BLSL. The result implies that some of the BLSL-related traps are quite stable at room temperature and could be used for geological dating. In addition, two paramagnetic centers produced by sudden release of high pressure in synthesis process were found in the unirradiated stishovite by electron spin resonance (ESR). Their g-factors are g=2.00181 and g=2.00062 for an axial signal and g=2.00305 for the other isotropic signal. These signals could be used for an evidence of impacts if those signals could be stored in geological time.     

Real-time luminescence from Al2O3 fiber dosimeters

The real-time luminescence signal from Al₂O₃ single crystal fibers, monitored during simultaneous irradiation and optical stimulation, was investigated using computer simulations and experimental measurements. Both radioluminescence (RL) and optically stimulated luminescence (OSL) signals were studied. The simulations were performed initially using a simple one-trap/one-recombination-center energy band model, and then extended to include shallow and deep electron traps as well. Real-time luminescence experiments were performed for different radiation dose rates and optical stimulation powers using periodic laser stimulation of the samples through a fiber optic cable, and the experimental results were compared with the predictions from the computer simulations. The luminescence signal was observed, both theoretically and experimentally, to increase from its initial value to a steady-state level. The steady-state RL and OSL levels were found to be dependent on dose rate, the steady-state level of the real-time OSL being independent of laser power. It was also shown that the total integrated absorbed dose throughout the irradiation period can be determined by correcting the real-time OSL signal for depletion caused by each laser stimulation pulse. The effects of the shallow and deep traps on the time-dependence of the real-time luminescence signal were studied comparing the experimental data from several Al₂O₃ fibers known to have different trapping state concentrations. The additional traps were found to slow the response of the real-time luminescence such that the time to reach steady state was increased as the additional traps were added.     

Monte Carlo simulations of luminescence processes under quasi-equilibrium (QE) conditions

Previous researchers have carried out Monte Carlo simulations of thermoluminescence (TL) phenomena by considering the allowed transitions of charge carriers between the conduction band, electron traps and recombination centers. Such simulations have demonstrated successfully the effect of trap clustering on the kinetics of charge carriers in a solid, and showed that trap clustering can significantly change the observed luminescence properties. While such Monte Carlo simulations have been carried out for TL, there has been no such trap clustering studies for optically stimulated luminescence phenomena (OSL). This paper presents a simplified method of carrying out Monte Carlo simulations for TL and linearly modulated optically stimulated luminescence (LM-OSL) phenomena, based on the General One Trap (GOT) model, which is a special case of the one trap one recombination center model (OTOR) when quasi-equilibrium conditions (QE) hold. The simulated results show that the presence of small clusters consisting of a few traps in a solid can lead to multiple peaks in both the TL and LM-OSL signals. The effects of retrapping and degree of trap filling are simulated for such multi-peak luminescence signals, and insight is obtained into the mechanism producing these peaks. The method presented in this paper can be easily generalized for other types of luminescence solids in which the recombination probability varies with time.     

不同退火温度的Al_2O_3:C薄膜热释光和光释光性能

α-Al_2O_3:C晶体的热释光和光释光性能优越,但其制备要求高,需高温和高还原气氛.与α-Al_2O_3:C晶体性能接近的α-Al_2O_3:C陶瓷,热释光峰不单一.本文采用两次阳极氧化法在0.5 mol/L的草酸溶液中5℃恒温制备高度均匀有序的多孔Al_2O_3:C薄膜,主要研究不同退火温度对其热释光和光释光特性的影响.结果表明,经不同温度退火后的Al_2O_3:C薄膜均为非晶结构;不同退火温度的Al_2O_3:C薄膜热释光的主发光峰约在310℃左右,符合通用级动力学模型.600℃退火后的Al_2O_3:C薄膜热释光灵敏度最强,其热释光剂量曲线在1-10 Gy范围内具有很好的线性响应,在剂量10-120 Gy范围内出现超线性响应;在相同的辐照剂量下,随着退火温度的升高(≤600℃)光释光的初始发光强度逐渐增强.不同退火温度的Al_2O_3:C薄膜光释光衰减曲线都呈典型的指数衰减且快衰减速率相比α-Al_2O_3:C晶体显著加快.600℃退火后的Al_2O_3:C薄膜光释光灵敏度最强,其光释光剂量响应曲线在1-200 Gy整体上都具有很好的剂量线性关系.与热释光相比,Al_2O_3:C薄膜的光释光具有更宽的线性剂量响应范围.此研究为Al_2O_3:C薄膜作为光释光辐射剂量材料做出了有益的探索.     

Photon dosimetry methods outside the target volume in radiation therapy: Optically stimulated luminescence (OSL), thermoluminescence (TL) and radiophotoluminescence (RPL) dosimetry

Dosimetry methods outside the target volume are still not well established in radiotherapy. Luminescence detectors due to their small dimensions, very good sensitivity, well known dose and energy response are considered as an interesting approach in verification of doses outside the treated region. The physical processes of thermoluminescence (TL), radiophotoluminescence (RPL) and optically stimulated luminescence (OSL) are very similar and can be described in terms of the energy band model of electron-hole production following irradiation.This work is a review of the main dosimetric characteristics of luminescence detectors which were used in experiments performed by EURADOS Working Group 9 for in-phantom measurements of secondary radiation (scattered and leakage photons). TL LiF:Mg,Ti detectors type MTS-7 (IFJ PAN, Poland), types TLD-100 and TLD-700 (Harshaw), OSL Al₂O₃:C detectors type nanoDot™ (Landauer Inc.) and RPL rod glass elements type GD-352M (Asahi Techno Glass Coorporation) are described. The main characteristics are discussed, together with the readout and calibration procedures which lead to a determination of absorbed dose to water.All dosimeter types used show very good uniformity, batch reproducibility and homogeneity. For improved accuracy, individual sensitivity correction factors should be applied for TL and OSL dosimeters while for RPL dosimeters there is no need for individual sensitivity corrections.The dose response of all dosimeters is linear for a wide range of doses.The energy response of GD-352M type dosimeters (with Sn filter) used for out-of-field measurements is flat for medium and low energy X-rays.The energy dependence for TLDs is low across the range of photon energies used and the energy correction was neglected. A significant over response of Al₂O₃:C OSLDs irradiated in kilovoltage photon beams was taken into account. The energy correction factor f_en was calculated by using the 2006 PENELOPE Monte Carlo code.With suitable calibration, all dosimeter types are appropriate for out-of-field dose measurements as well as for the in-phantom measurements of radiotherapy MV X-rays beams.     

LiMgPO_4:Tm,Tb的热释光和光释光陷阱参数

采用高温固相法合成了LiMgPO_4:Tm,Tb粉末样品,测定了热释光陷阱参数激发能E和频率因子s.用脉冲退火和多次退火方法研究了其光释光陷阱参数E和s,并与用多速法得到的热释光的结果进行了比较.对不同β射线剂量照射的样品发光曲线的研究表明,300°C高温峰属于一级动力学发光峰.通过对热释光和光释光陷阱的相关性研究表明,经200°C预热的热释光信号(对应于300°C高温峰)和光释光信号很有可能来自于同一深度的陷阱.     

Review of optically stimulated luminescence (OSL) instrumental developments for retrospective dosimetry

This review describes 40 years of experience gained at Risø National Laboratory in the development of facilities for irradiation, thermal/optical stimulation and luminescence signal detection. These facilities have mainly been used in luminescence dating and nuclear accident dosimetry. We focus especially on methods for light stimulation and irradiation, and developments of new portable TL/OSL readers for determining doses directly in the field on both Earth and the planet Mars.     

Thermoluminescence and optically stimulated luminescence disadvantages of α-Al2O3:C crystal grown by the temperature gradient technique

Recently, α-Al₂O₃:C crystal with highly sensitive thermoluminescence (TL) and optically stimulated luminescence (OSL) has been successfully grown by the temperature gradient technique. This paper investigates the heating rate dependence of TL sensitivity, light-induced fading of TL signals and thermal stability of OSL of α-Al₂O₃:C crystals. As the heating rate increases, the integral TL response decreases and the dosimetric glow peak shifts to higher temperatures in α-Al₂O₃:C crystals. Light-induced fading of TL increases with the irradiation dose, and TL response decreases as the exposure time increases, especially in the first 15 minutes. With the increasing intensity of the exposure light, the TL fading of α-Al₂O₃:C crystal increases sharply. The OSL response of as-grown α-Al₂O₃:C crystal is quite stable below 373 K and decreases sharply for higher temperatures.     

Relative response of TL and component-resolved OSL to alpha and beta radiations in annealed sedimentary quartz

Knowledge of the relative luminescence response to alpha and beta radiation is very important in TL and OSL dating. In the present study the relative alpha to beta response is studied in a sedimentary quartz sample, previously fired at 900 °C for 1 h, in the dose region between 1 and 128 Gy, for both thermoluminescence (TL) and linearly modulated optically stimulated luminescence (LM – OSL). The LM – OSL measurements were performed at room temperature and at 125 °C. All OSL signals were deconvolved into their individual components. Comparison of OSL curves after alpha and beta irradiation strongly supports that quartz OSL components follow first order kinetics in both cases. In the case of TL, the relative alpha to beta response is found to be very different for each TL glow-peak, but it does not depend strongly on irradiation dose. In the case of LM – OSL measurements, it is found that the relative behaviour of the alpha to beta response is different for three distinct regions, namely the fast OSL component, the region of medium OSL component originating from the TL glow-peak at 110 °C when stimulation takes place at room temperature and finally the region of slow OSL component. Following stimulation at ambient temperature, the relative alpha to beta response of all components was not observed to depend significantly on dose, with the value of ratio being 0.03 and a tendency to decrease with increasing dose. However, in the case of measurements performed at 125 °C, the relative response of the fast components is much enhanced, and for the remaining components it increases with increasing dose. Special care must be taken to examine the relative alpha to beta response of the fast component at 125 °C which contrasts the relative response of the TL peak at ca. 325 °C. The implications for the dating of annealed quartz are also briefly discussed.     

SrSO4:Eu磷光体的光释光特性

研究了通过掺杂得到的SrSO4:Eu(01mol%)的粉末样品的光释光(OSL)特性.用90Sr的β射线辐照0116—116kGy后，测定了恒定光源激发的光释光发光曲线(CW-OSL)和线性光源激发的光释光发光曲线(LW-OSL)，对发光曲线分析均得到了四种陷阱成分.采用复合作用响应函数得到SrSO4:Eu辐射剂量响应为线性-亚线性.测量了温度对OSL信号的影响，结果表明OSL信号的温度稳定性很好，最灵敏读出温度约为180℃，说明这时OSL信号来自热激发和光激发的共同作用.用60Coγ辐照100Gy后，测量了热释光(TL)三维光谱，确定了发光波长主要位于375nm，可以确定这是来自于Eu2+能级跃迁的发光. 关键词： 光释光 热释光 SrSO4:Eu     

OSL and TL retrospective dosimetry with a fluorapatite glass-ceramic used for dental restorations

Optically Stimulated Luminescence (OSL) and Thermoluminescence (TL) properties of a fluorapatite glass-ceramic have been investigated, with a view to developing a dose assessment technique for medical triage following unplanned exposures of individuals to ionizing radiation. The ceramic is an innovative material used in dental prostheses and restorations. It is strongly sensitive to radiation and the intensity of both the OSL and TL signals are proportional to the absorbed radiation dose. We focused on the optimization of the measuring procedure and investigated characteristics such as reproducibility, fading, minimum detectable dose (MDD), dose response and photon energy response of TL and OSL signals. The dental ceramic exhibited very good reproducibility (<5% at 2σ level) when measured and a linear dose response for a wide range of doses (50 mGy–20 Gy). The MDD values for the samples investigated were ∼5 mGy. The material is not tissue equivalent and the OSL and TL signals are strongly dependent on incident photon energy. Both the luminescence signals exhibited significant fading during the first few hours after irradiation. Its rate was dependent on the parameters of measurement. The results indicate that the material can be used for the purposes of accident dosimetry, however, the fading and photon energy response have to be properly corrected for a reliable dose assessment.     

Comparison of the properties of various optically stimulated luminescence signals from potassium feldspar

Various optically stimulated luminescence signals from K-feldspar have been used to determine the equivalent doses of sediment samples. Understanding the properties of these optical signals is critical to evaluate their applicability and limitations to optical dating. In this paper, some properties of IRSL, post-IR OSL and post-IR IRSL signals (detected in the UV region using U-340 filters) from a museum sample of K-feldspar were investigated by analyzing the relationships between optical and TL signals, and the effect of optical bleaching and heating on optical signals. The trap parameters of the different optical signals were calculated using the pulse annealing method. The results show that this sample exhibits two regenerated TL peaks at ～140 and ～330 °C. Corresponding to the low temperature TL peak, the OSL and post-IR OSL signals appear to be more associated with lower temperature TL than the IRSL signal measured at 50 °C. Corresponding to the high temperature TL peak, the post-IR IRSL signals mainly originate from the more thermally stable traps associated with the high temperature TL, compared with the IRSL and post-IR OSL signals. However, the post-IR IRSL_225 °C signal is shown to be hard to be bleached by blue light and simulated sunlight, compared with the IRSL_50 °C and low temperature post-IR IRSL signals. The implication for optical dating is that the elevated temperature post-IR IRSL signals can be preferentially applied over other signals from K-feldspar, but it is desirable that the effectiveness of the pre-depositional zeroing of these signals is assessed.     

Spectral information from minerals relevant for luminescence dating

The paper reviews basic spectral features of luminescence from minerals used in dating and allied research. Luminescence production is a result of multiple interactions within the imperfect crystal lattice and spectral information is not limited to the emission of light. Results of spectral investigations of luminescence emission during thermal stimulation (TL) or optical stimulation (OSL) form the main part of the paper. However, information on luminescence excitation and light absorption spectroscopy is also presented and possible links between luminescence production in minerals and particular lattice defects are considered. Quartz and feldspars, the most commonly used minerals, receive special attention, but the review includes other materials such as polymineral fine-grained fractions from sediments, zircon, calcite and other salts (halite, sulfate), meteorites, flint, volcanic materials (obsidian, tephra), ceramics and metallurgical slags. Although a wide range of different luminescence emission wavebands occur, it can be shown that certain emissions dominate in particular materials. Basic dosimetric properties are often known just for single emission wavebands of a particular mineral, and are listed in this case. The paper also aims to provide a starting point and inspiration for the study of other TL and OSL emissions, with particular regard to their potential and suitability for dating and related dosimetry tasks. These investigations, involving palaeodose determination based on an emission waveband with known characteristics, need careful separation of the particular emission peak, which may be influenced by its behaviour during the dating procedure (sample preparation, irradiation, preheat treatments, luminescence measurements, etc.). Spectral information available in this context and some technical remarks on the experimental conditions will be given to pave the way for conventional TL or OSL measurements in luminescence dating and dosimetry using natural or semi-natural materials.     

Monte Carlo simulations of TL and OSL in nanodosimetric materials and feldspars

The study of luminescent materials consisting of nanoclusters is an increasingly active research area. It has been shown that the physical properties of such nanodosimetric materials can be very different from those of similar conventional microcrystalline phosphors. In addition, it has been suggested that traditional energy band models may not be applicable for some of these nanodosimetric materials, because of the existence of strong spatial correlations between traps and recombination centers. The properties of such spatially correlated materials have been previously simulated by using Monte Carlo techniques and by considering the allowed transitions of charge carriers between the conduction band, electron traps and recombination centers. This previous research demonstrated successfully the effect of trap clustering on the kinetics of charge carriers in a solid, and showed that trap clustering can significantly change the observed luminescence properties. This paper presents a simplified method of carrying out Monte Carlo simulations for thermoluminescence (TL) and optically stimulated luminescence (OSL) phenomena, based on a recently published model for feldspar. This model is based on tunneling recombination processes involving localized near-neighbor transitions. The simulations show that the presence of small clusters consisting of a few traps can lead to multiple peaks in both the TL and linearly modulated OSL signals. The effects of donor charge density, initial trap filling and cluster size are simulated for such multi-peak luminescence signals, and insight is obtained into the mechanism producing these peaks.     

Correlation of optically and thermally stimulated luminescence of natural fluorite pellets

Natural fluorite (CaF₂), a dosimetric material of large usage, presents Thermoluminescence (TL) and Optically Stimulated Luminescence (OSL). This study examined the behavior of TL and OSL (stimulated with Blue LEDs) signals from the Brazilian natural fluorite pellets with NaCl as binding agent, as well as their correlations, in order to study and optimize the dosimetric process with this material. A series of experiments were conducted, basically with thermal treatments before OSL acquisition, and optical bleaching before TL readout. The role of NaCl in the TL and OSL emission was investigated. It was observed that natural CaF₂ TL signal is still ample to be used in dosimetric applications, as dose re-assessment in personal dosimetry after an OSL measurement. Also it was verified that the fluorite OSL signal is extinguished by a 350 °C heating and that NaCl has no contribution to the stable part of the OSL signal.     

Dose-dependent optically stimulated luminescence of synthetic quartz at room temperature

Physical conditions such as annealing temperature, duration of annealing, ionizing radiation, etc., play a significant role in the applications of optically stimulated luminescence (OSL) dating as well as OSL dosimetry. Many efforts are made to understand the effect of these physical parameters on quartz specimens owing to its use in such applications. Such factors induce changes in OSL decay pattern. The definite correlation between color centers and luminescence sensitivity can be established on account of such pre-treatments to the specimen.The purpose of present investigations is to study the effect of ionizing radiation under identical physical conditions on OSL properties measured at room temperature. The shapes of decay curve and dose-response data are considered for this purpose. This study can reveal the changes in color centers in response to the pre-conditions to the specimen. It was found that the OSL decay remains slow and OSL properties change systematically with the rise in beta dose up to a critical dose; however, it changes the pattern when the beta exposure to the specimen was increased higher than the critical dose. This critical dose was found to be different for different temperature of annealing. The shape of decay curve up to the critical dose was also studied by considering the difference of OSL intensities between two successive durations from the observed OSL decay data. The results are explained based on the changes in available shallow traps during OSL measurement at room temperature with changes in pre-conditions to the specimens. The results also have been confirmed with the corresponding changes in ESR signals.