Superlinear dose response of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals in luminescence materials: An analytical approach

The phenomenon of superlinear dose response of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals has been reported for several important dosimetric materials. We develop new analytical equations for the filling of traps and centers during irradiation and for the read-out stage of annealed luminescence materials, within the context of a two-trap and two-center model. The equations are applicable for both TL and OSL signals in annealed dosimetric materials, and are derived under the assumptions of low irradiation doses and dominant strong retrapping (weak recombination) processes. For low doses all traps and centers display linear dose response, which leads to quadratic dose response of the integrated TL/OSL signals. A new analytical expression is presented for this well-known quadratic dose dependence, in terms of the kinetic parameters in the model. The effect of elevated irradiation temperature on the integrated TL/OSL signals is also considered, and analytical expressions are obtained for this situation as well. A new type of dose-rate effect is reported based on the modeling results, which is due to irradiation during elevated temperatures. The accuracy of the analytical expressions is verified by comparing with the results of numerical simulations.     

A new look at the linear-modulated optically stimulated luminescence (LM-OSL) as a tool for dating and dosimetry

Optically stimulated luminescence (OSL) has been in use for dosimetry and dating in the last two decades. Since the OSL dependence on time is a featureless decaying function, a linear-modulation of the stimulating-light intensity has been suggested [Bulur, E., 1996. An alternative technique for optically stimulated luminescence. Radiat. Meas. 26, 701–709.], which resulted in a peak-shaped curve. The properties of this curve have been studied, assuming first-, second- and general-order kinetics. In a recent paper we have shown [Chen, R., Pagonis, V., 2008. A unified presentation of thermoluminescence (TL), phosphorescence and linear-modulated OSL (LM-OSL). J. Phys. D: Appl. Phys. 41, 035102 (1–6).] that for general-order curves, the peak maximum cannot be expected to depend linearly on the dose of excitation. A new presentation of the LM-OSL has been suggested, in which the peak maximum is linear with the filling of trapping states, which, in turn, may be expected to be linear with the dose under appropriate conditions. In the present work, we report on results of numerical simulation of the LM-OSL using the one trap-one recombination center (OTOR) model, dealing with the traffic of carriers between one trapping state, one kind of recombination center and the conduction and valence bands during excitation and read-out, and without making any simplifying assumptions. The process during optical read-out has been followed in the simulation that consisted of the numerical solution of the relevant sets of coupled differential equations, and also by analytical treatment. Sets of parameters leading to approximately first- and second-order kinetics, and to intermediate cases, have been used and the results presented in the original and the new ways are shown. The consequences concerning dating and dosimetry are discussed.     

Nonlinear dose dependence of TL and LM-OSL within the one trap-one center model

In a recent paper, it has been shown that strong sub-linearity of the occupancy n₀ of trapping states far from saturation can be explained by the simplest model of one trap-one recombination center (OTOR). In the present work we report on results of numerical simulation of dose dependence of the TL maximum under similar conditions. In some cases, the TL maximum is found to be strictly proportional to the filling of the traps, but this is not always the case. Different sublinear dose-dependence functions of the trap occupancy and the maximum TL are demonstrated. With the same sets of parameters, curves of LM-OSL have also been simulated; superlinear as well as sublinear dependencies on the excitation dose have been found.     

Development of a new curve deconvolution algorithm for optically stimulated luminescence

A new computerized glow curve deconvolution (CGCD) algorithm for thermoluminescence(TL) and optically stimulated luminescence (OSL) is presented. The proposed approach can be adopted in a numerical curve fitting for obtaining the relevant trapping parameters of a set of glow data taken with both thermal and optical stimulation. This method is based on the one trap one recombination center (OTOR) model with minimal simplifying assumptions. To demonstrate the ability of the method, a new computer program has been developed and tested with some synthetic OSL data.     

The role of simulations in the study of thermoluminescence (TL)

The traffic of charge carriers in a luminescent material during its excitation by irradiation and during readout either in the measurement of thermoluminescence (TL) or optically stimulated luminescence (OSL) is governed by sets of coupled nonlinear differential equations. The analytical solution of these sets is usually not possible, and one can resort to one of two options. Some researchers preferred to make simplifying assumptions and thus got approximate solutions whereas others performed simulations by solving the simultaneous equations numerically. Each of these routes has its pitfalls. The simplifying assumptions, mainly the quasi-equilibrium assertion or the assumption that certain relations between the relevant parameters and functions hold, may be valid in certain ranges of the TL or OSL curve, and may cease to be valid, say at the high-temperature range in TL. Performing simulations using the numerical solution of the relevant set of equations may yield results which are accurate, but cannot be considered as being general because they depend on the specific choice of the parameters. Repeating the simulations with several sets of the physically plausible parameters would add credibility to the conclusions drawn. The combination of the two approaches is highly recommended, i.e, if similar results are found by approximations and simulations, the validity of the conclusions is strengthened. Evidently, the comparison of these theoretical results to experimental effects is essential. In the present work we consider the occurrence of unusually high and unusually low values of the activation energy and the effective frequency factor. In particular, we can simulate a recently discovered behavior of TL in LiF:Mg, Cu, P at the ultra-high dose range and get qualitatively the main elements of the experimentally found results.     

Non-monotonic dose dependence of the Ge- and Ti-centres in quartz

The dose response of the Ge- and Ti-centres in quartz is studied over a large dose range. After an initial signal increase in the low dose range, both defects show a pronounced decrease in signal intensities for high doses. The model by Euler and Kahan [1987. Radiation effects and anelastic loss in germanium-doped quartz. Phys. Rev. B 35 (9), 4351–4359], in which the signal drop is explained by an enhanced trapping of holes at the electron trapping site, is critically discussed. A generalization of the model is then developed, following similar considerations by Lawless et al. [2005. A model for non-monotonic dose dependence of thermoluminescence (TL). J. Phys. Condens. Matter 17, 737–753], who explained a signal drop in TL by an enhanced recombination rate with electrons at the recombination centre. Finally, an alternative model for the signal decay is given, based on the competition between single and double electron capture at the electron trapping site. From the critical discussion of the different models it is concluded that the double electron capture mechanism is the most probable effect for the dose response.     

Evaluated thermoluminescence trapping parameters–What do they really mean?

The main two trapping parameters in thermoluminescence (TL), the activation energy and the frequency factor, are often calculated and used for the evaluation of the stability of the TL signal at a given temperature. In several cases, “anomalous” values of these parameters, either very high or very low have been reported in the literature. In practically all of these cases, the values reported have been recognized to be effective values which resulted from some special circumstances related to the specific materials in hand. Obviously, these effective values are not associated directly with the real rate of thermal release of carriers from traps at the ambient temperature, prior to heating, and therefore, they do not indicate the real decay time of the TL signal or, in other words, the stability of the signal which may be used in TL dosimetry or dating of archaeological or geological samples. In the present paper, we discuss briefly some of these cases and add, in more detail, a rather elementary situation of very low effective activation energy and frequency factor. A model with two trapping states and one kind of recombination center is used and the simulation includes the numerical solution of the relevant sets of coupled differential equations in the three stages of the measurement, namely, excitation, relaxation and heating for a given set of the trapping parameters. The parameters are chosen in such a way that two overlapping TL peaks occur, which look together like a single first-order peak, but with anomalously low evaluated effective activation energy and frequency factor. Implications regarding the possible results in glow curve deconvolution are discussed.     

Dependence of the anomalous fading of the TL and blue-OSL of fluorapatite on the occupancy of the tunnelling recombination sites

The anomalous fading (AF) of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals in Durango apatite is attributed to tunnelling effects. Electrons from the TL and OSL traps in this material are transferred, via a tunnelling effect, to the recombination sites. The availability of recombination sites for tunnelled electrons is of major importance for the degree of AF rate observed in this material. It is expected that a variation of the number of the electron recombination sites will be reflected in the experimentally measured AF rate. In the present work an investigation of the recombination sites for the tunnelled electrons is attempted by studying the AF effect using a special technique, in which the anomalously faded TL (OSL) is replaced by an equal amount of TL (OSL) induced by a beta dose.     

Monitoring environmental dose rate using Risø TL/OSL readers with built-in sources: recommendations for users

Measurements were carried out to quantify the dose rate delivered to samples due to leakage and cross-talk of the beta and alpha sources in various models of Risø TL/OSL readers; additionally the offset time was calculated. Highly sensitive -Al₂O₃:C and CaF₂:Mn dosemeters were used to investigate the impact on low environmental dose-rate assessment. The effect is shown to depend on the energy response of the detectors, the source strength and the reader design of the equipment. It was tested, if the scattered radiation of the closed source can be utilised to extend the dose range downwards to lower doses, as the dose rates of the built-in sources of Risø TL/OSL readers often exceed the practical values for ultra-low-dose measurements. The results and their consequences for environmental dose-rate assessment are discussed.     

Nanodosimetric kinetic model incorporating localized and delocalized recombination: Application to the prediction of the electron dose response of the peak 5a/5 ratio in the glow curve of LiF:Mg,Ti (TLD-100)

A kinetic model combining both localized and delocalized recombination is described which is based on different filling rates as a function of irradiation electron energy of a spatially correlated trapping center/luminescent center (TC/LC) complex. Following irradiation and thermal de-trapping the locally trapped electron-hole configuration is assumed to give rise to peak 5a and the e-only configuration to peak 5 in the glow curve of LiF:Mg,Ti (TLD-100). The model is capable of simulating the linear/supralinear dose response of composite peak 5, the dependence of the supralinearity on photon energy and the ratio of the intensities of peak 5a to peak 5 as a function of dose. However, this is achieved only by invoking the presence of band-tail states which allow thermally induced hopping leading to semi-localized recombination in the recombination mechanism of the e-only configuration.     

Testing a model-guided approach to the development of new thermoluminescent materials using YAG:Ln produced by solution combustion synthesis

The objective of this work is to test a model-guided approach, coupled with an efficient material synthesis method, for the development of new thermoluminescent (TL) material using yttrium aluminum garnet (YAG, Y₃Al₅O₁₂) as a model material. We systematically investigated undoped and lanthanide-doped YAG using x-ray diffraction (XRD), TL, and radioluminescence (RL) to understand the role of the lanthanides in the TL process, i.e., whether they act as trapping centers or recombination centers. We also prepared samples with multiple dopants to test the possibility of creating materials with multiple TL peaks. The initial rise method of TL analysis was used to estimate the activation energies associated with the TL peaks.The role of the lanthanide impurities predicted using the lanthanide energy level diagram was largely confirmed, as evidenced by the TL curves, TL emission spectra and activation energy analysis. However, our data suggests that the exact role of the lanthanide dopants during the TL process depends on the thermal stability of the trapped charges, i.e. the same lanthanide can act as a trapping center in one system and as a recombination center in another system. These results demonstrate the possibility of introducing appropriate TL peaks and recombination centers in YAG produced by SCS by lanthanide doping, where the role of the lanthanide dopant is consistent with a model for the lanthanide energy levels. This allows for a more guided approach to the development of new TL materials with peaks in certain temperature range or multiple TL peaks, at least in conditions in which the model applies.     

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.     

Applicability of OSL pre-dose phenomenon of quartz in the estimation of equivalent dose

The feasibility of utilizing the pre-dosed OSL signal in the estimation of the equivalent dose has been investigated. The results based on (i) the behavior of growth curve, (ii) dose recovery tests and (iii) non-bleachability of reservoir centres, R-centres, suggests that (i) the pre-dosed OSL does not seem to work satisfactorily in dose estimation unlike the pre-dosed 110 °C TL emission and (ii) it may not be applicable in case of bleached specimen.     

OSL and TL in TLD-100 following alpha and beta irradiation: Application to mixed-field radiation dosimetry

The optically stimulated luminescence (OSL) of LiF:Mg,Ti (TLD-100) following irradiation by beta and alpha particles was investigated by measurement of the excitation and emission spectra of OSL and comparison with thermoluminescence (TL) characteristics. The OSL excitation spectra of all the samples following both beta and alpha irradiation are very similar.Identical emission bands with very similar relative intensities following both beta irradiation and alpha particle irradiation have been recorded in the OSL induced in nominally pure LiF mono and TLD-100 polycrystals. The identical excitation and emission bands in the doped and pure crystals are strong evidence indicating that the observed OSL is due to an intrinsic trapping structure. The OSL has indeed been previously attributed to F₂ centers and F₃⁺ centers.The preferential excitation of OSL compared to TL following high ionisation density (HID) alpha irradiation is naturally explained via the identification of OSL with the “two-hit” F₂ or F₃⁺ center, whereas the major component of composite TL glow peak 5 is believed to arise from a “one-hit” complex defect. This discovery allows near-total discrimination between HID radiation and low ionisation density (LID) radiation and may have significant potential in mixed-field radiation dosimetry.     

A computer program for the deconvolution of the thermoluminescence glow curves by employing the interactive trap model

An efficient computer program has been developed to deconvolute thermoluminescence (TL) glow peaks and optically stimulated (OSL) curves by employing a method of the interactive trap model (ITM). The program is designed to be used easily on the MS Windows-based computer with a graphical user interface. This program could be used to analyze the TL glow curves by using the traditional first-order kinetics (1OK), second-order kinetics (2OK), general order kinetics (GOK), mixed order kinetics (MOK) and the general approximation (GA) method as well as ITM. The program was tested with the generated data and the experimental results of deconvoluted TL glow curves of LiF TLD-100 by assigning five interacting traps and one recombination center. A complete version with full functionalities of this program can be downloaded from the web site http://physica.gnu.ac.kr/TLanal.     

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.     

Further investigations of tunneling recombination processes in random distributions of defects

The shape of infrared stimulated luminescence signals (IRSL) from feldspars has been the subject of numerous studies in the field of luminescence dating. Specifically linearly modulated IRSL signals (LM-IRSL) are commonly assumed to consist of several first order components corresponding to distinct optical stimulation cross sections. This paper models the shape of LM-IRSL signals using a recently proposed kinetic model, which describes localized electronic recombination in donor–acceptor pairs of luminescent materials. Within this model, recombination is assumed to take place via the excited state of the donor, and nearest-neighbor recombinations take place within a random distribution of centers. The model has been used previously successfully to describe both thermally and optically stimulated luminescence (TL, OSL). This paper shows that it is possible to obtain approximate solutions for the distribution of donors in the ground state as a function of two variables, time and the distance between donors and acceptors. Approximate expressions are derived for several possible modes of optical and thermal stimulation, namely TL, OSL, linearly modulated OSL (LM-OSL), LM-IRSL and isothermal TL (ITL). Numerical integration of these expressions over the distance variable yields the distribution of remaining donors at any time t during these experimental situations. Examples are given for the derived distributions of donors in each experimental case, and similarities and differences are pointed out. The paper also demonstrates how LM-IRSL signals in feldspars can be analyzed using the model, and what physical information can be extracted from such experimental data. The equations developed in this paper are tested by fitting successfully a series of experimental LM-IRSL data for Na- and K-feldspar samples available in the literature. Finally, it is shown that the equations derived in this paper are a direct generalization of an equation previously derived for the case of ground state tunneling.     

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.     

Nanostructured layers of anion-defective gamma–alumina – New perspective TL and OSL materials for skin dosimetry. Preliminary results

Thin- layer material based on nanostructured Al₂O₃ of the surface density 5 mg/cm² was obtained. The material is characterized by high OSL and TL yields comparable with those for TLD-500 which is one of the leaders among the TL and OSL detectors. The dose response, fading and dependence of TL yield on heating rate was studied. It is established that high luminescence yield of the samples under study correlates with the content of anion vacancies and γ-phase of Al₂O₃. The data for time-resolved luminescent spectroscopy are presented, which evidence for possible correlation between high TL and OSL activity and the F-type centers. It is noted that the material needs to be modified for successful use in dosimetry. In addition further studies to decrease the contribution of unstable (at 300 К) components to OSL and TL yields are required.     

不同粒径α-Al2O3:C晶态粉体热释光和光释光特性

本文探讨了α -Al₂O₃:C晶态粉体的辐照剂量效应, 使用RisøTL/OSL-DA-15 型热释光和光释光仪研究其热释光和光释光特性, 结果发现, 相同粒径的α-Al₂O₃:C晶态粉体具有单一热释光峰, 且随着辐照剂量的增加热释光强度不断增加, 但热释光峰位置保持不变, 符合一级动力学模型; 而在相同的辐照剂量和测试条件下, 随着α -Al₂O₃:C晶态粉体粒径的减小, 其热释光强度先增强后减弱, 热释光峰却逐渐增加至趋于稳定, 表明粒度为40—60 μ的α -Al₂O₃:C晶态粉体具有最佳的热释光效应. 同时α -Al₂O₃:C晶态粉体的光释光特性的研究发现, 其光释光曲线具有典型的指数衰减特征, 粒径对其光释光强度和衰减速率的影响符合浅电子陷阱能级理论.