Comparative investigations of TL and OSL in KCI:Eu2+ crystals irradiated with UV and X-rays

Abstract

We present thermoluminescence (TL) glow curves and optical stimulated luminescence (OSL) response from both KCl:Eu²⁺ crystals irradiated with soft X-rays (20 KV, 80 μA) and ultraviolet light (230 nm). Two situations take place. First, we observed that for long time F-light bleaching (560 nm) the typical TL glow curve of X-rays irradiated KCl:Eu²⁺ resembles the TL glow curve of UV-irradiated samples. Second, along with OSL measurements, we have performed a thermal bleaching and we have addressed F and F_z participation in OSL. These results provide us a supportable correlation between F and F_z as responsible centers for OSL and TL processes.     

An algorithm for unified analysis on the thermoluminescence glow curve

An algorithm was developed to integrally handle excitation by radiation, relaxation and luminescence by thermal or optical stimulation in thermoluminescence (TL) and optically stimulated luminescence (OSL) processes. This algorithm reflects the mutual interaction between traps through a conduction band. Electrons and holes are created by radiation in the beginning, and these electrons move to the trap through the conduction band. These holes move to the recombination center through a valence band. The ratio of the electrons allocated to each trap differs with the recombination probability and these values also relevant to the process of luminescence. Accordingly, the glow curve can be interpreted by taking the rate of electron–hole pairs created by ionizing radiation as a unique initial condition. This method differs from the conventional method of interpreting the measured glow curve with the initial electron concentration allocated to each trap at the end of irradiation. A program using the Visual Studio's C# subsystem was made to realize such a developed algorithm. To verify this algorithm it was applied to LiF:Mg,Cu,Si. The TL glow curve was deconvoluted with a model of five traps, one deep trap and one recombination center (RC).     

Modelling the optical bleaching of the thermoluminescence of K2YF5:Pr3+

Optical bleaching of the thermoluminescence (TL) curve of K₂YF₅:Pr³⁺ has been observed after optically stimulated luminescence (OSL) readout of pre-irradiated crystals. The traps being responsible for the TL signal are not emptied completely by the optical stimulation. Furthermore, if the illumination time is increased a constant intensity level of the residual TL glow curve is eventually achieved. On the other hand, if the low temperature peak of the glow curve is thermally cleaned, no subsequent OSL is measured. This behavior has been successfully explained by assuming that part of the electrons in the trap being responsible for the low temperature glow peak of K₂YF₅:Pr³⁺ recombine with holes via localized transitions during optical stimulation. During TL all trapped electrons recombine via delocalized transitions. Simulations have been carried out in order to demonstrate the feasibility of the model.     

Thermoluminescence dosimetry: State-of-the-art and frontiers of future research

The state-of-the-art in the use of thermoluminescence for the measurement of energy imparted by ionizing radiation is discussed. Emphasis is on the advantages obtainable by the use of computerized glow curve analysis in (i) quality control, (ii) low dose environmental dosimetry, (iii) medical applications (especially precision) and microdosimetric applications, and (iv) mixed field ionization-density–dosimetry. Possible frontiers of future research are highlighted: (i) vector representation in glow curve analysis, (ii) combined OSL/TL measurements, (iii) detection of sub-ionization electrons, (iv) requirements for new TL materials and (v) theoretical subjects involving kinetic modeling invoking localized/delocalized recombination applied to dose response and track structure theory including creation of defects.     

A new method for the numerical analysis of thermoluminescence glow curve

A new method to analyze the thermoluminescence (TL) glow curve has been presented. It has been shown that this method is efficient and fast in generating the TL glow curves and can be adopted in a numerical curve fitting for obtaining the relevant TL parameters of a given TL glow curve data. This new method is based on a general approximation (GA) which assumes only that the concentration of the electrons in the conduction band is negligible when compared with the concentration of the electrons in the traps. The GA method has been tested against the reference glow curve data which was generated by the full iteration method without any prior approximation in the one-trap-one-recombination-centre model. By finding the best fit between the reference data and the curves generated by the GA method, the values of the kinetics parameters have been determined. Also, the general order kinetics (GOK) and the peak shape method have been examined. The fitted values of the activation energy and the initial concentration of electron by the GA method match reasonably well with the original value.     

Thermal assistance in TA – OSL signals of feldspar and polymineral samples; comparison with the case of pure quartz

Thermally assisted optically stimulated luminescence (TA – OSL) is studied for the cases of polymineral, rich in K-feldspar sample as well as one pure sample of K-feldspar. For both cases, the shape of the TA – OSL signal indicates an initial, fast decaying part which is followed by a flat, very slowly decaying part with intensity much larger than the ordinary background noise signal. Thermal assistance characteristics indicate that for the case of pure K-feldspar, the signal originates from a unique very deep trap. The experimental features of the TA – OSL signal in the case of polymineral sample resemble much the corresponding TA – OSL features of pure quartz, in terms of both glow curve shape, especially at high stimulation temperatures, as well as signal intensity and its dependence on the stimulation temperature. Nevertheless, TA – OSL stimulation at low, ambient temperatures provide strong hints towards the contribution of K – feldspars to this signal. Proper selection of the stimulation temperature could possibly discriminate the TA – OSL signal originating from quartz and feldspars.     

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.     

Optical depth of traps in AL2O3:C determined by the variable energy of stimulation OSL (VES-OSL) method

Standard methods of OSL measurements (CW-OSL or LM-OSL) do not allow for the direct determination of optical depth of traps. The variable energy of stimulation optically stimulated luminescence (VES-OSL) method gives such possibility. It consists in optical stimulation with the continuous increase of stimulation light energy and is analogous to the glow curve method in TL measurements. The VES-OSL curve shape and maximum position can be regulated by the stimulation photon flux, the rate of stimulation energy increase and by measurement temperature. This allows for detecting the OSL from very deep traps that give the TL signal overlapping with strong incandescence. The VES-OSL measurements carried out for Al₂O₃:C showed that traps having the optical depth between 2.0 and 2.8 eV are responsible for the OSL signal related to TL peak at about 200 °C. The OSL signal from the much deeper traps from the range 2.8–3.3 eV was also detected. The TL signal related do these traps cannot be detected below 500 °C.     

Energy levels in YPO4:Ce3+,Sm3+ studied by thermally and optically stimulated luminescence

Energy-resolved optically stimulated luminescence (OSL) spectra and thermoluminescence (TL) glow curves of a powder sample of YPO₄:Ce³⁺,Sm³⁺ were measured to investigate the nature of the trapping centre and to locate its energy level relative to the valence and conduction bands of the YPO₄ host. The high-temperature glow peak could unequivocally be assigned to Sm²⁺ (thus Sm³⁺ acts as an electron trap). The trap depth of this centre, as derived from the OSL excitation spectra, is in good agreement with the Dorenbos model prediction. The OSL excitation spectra also reveal excited states of Sm²⁺ well below the conduction band. These excited states produce a broadening of the high-temperature TL glow peak and also cause the activation energy determined by the Hoogenstraten method to underestimate the trap depth.     

Thermally assisted OSL from deep traps in Al2O3:C

The present work suggests an alternative experimental method in order to not only measure the signal of the deep traps in Al₂O₃:C without heating the sample to temperatures greater than 500 °C, but also use this signal for high dose level dosimetry purposes as well. This method consists of photo transfer OSL measurements performed at elevated temperatures using the blue LEDs (470 nm, FWHM 20 nm) housed at commercial Risø TL/OSL systems, after the sample was previously heated up to 500 °C in order to empty its main TL dosimetric trap. The influence of this procedure on specific features such as glow curve shape and sensitivity of the main TL glow peak was also studied.     

OSL from BeO ceramics: new observations from an old material

In BeO ceramics, exposed to ionizing radiation, an intense OSL signal was observed. The properties of the signal and its behavior under various experimental conditions were investigated. It was found that the OSL signal is a composite signal and exhibits strong thermal quenching. The quenching energy was estimated as 0.5 eV. The excitation spectrum of the OSL signal was obtained as a broad peak in the region 420–550 nm with maximum around 435 nm. The possible correlation between the OSL signal and the peaks in the TL glow curve was also examined. It was interesting to observe that the highly light sensitive TL peak near 220°C does not contribute to the OSL signal. The OSL signal was found to originate from a trap near 340°C.

To check the possibility of using the material for radiation dosimetry the dose response and thermal stability of the OSL signal were also investigated. The dose response was found to be quite linear up to 10 Gy. The thermal activation energy of the OSL trap was determined as 1.7 eV using isothermal annealing and heating rate methods thus proving the suitability for dosimetry.     

Characteristics of LM-OSL from several different types of quartz

We present Linear-Modulation OSL (LM-OSL) curves from several different types of quartz, including sedimentary quartz, bulk rock crystal and synthetic quartz. The LM-OSL method consists of linearly increasing the intensity of the stimulation light while continuously monitoring the OSL emission from the sample. With this technique, one obtains peaks of luminescence intensity versus time (Bulur, 1996) in which the position of the peak is inversely related to the photoionization cross-section of the trap. The shape of the LM-OSL curve is directly related to the shape of the conventional OSL decay curve in which the stimulating light source is maintained at constant intensity (so-called Continuous-Wave OSL, or CW-OSL). In the latter, the OSL from the traps with the highest photoionization cross-section decays most rapidly with stimulation time, while OSL from those traps with smaller photoionization cross-sections is characterized by longer decay times. In this paper, data are presented comparing the CW-OSL and LM-OSL curves for several different quartz types with particular focus on the changes in the shapes of each of these curves with sample type pre-heat temperature, and measurement temperature. Several different LM-OSL components are found for each sample, each with different photoionization cross-sections, but a universal behavior for quartz is not observed; each sample is different. From the dependence upon pre-heat temperature, features associated with shallow traps can be identified. Traps which empty very rapidly can be observed more easily in the LM-OSL curves than in the conventional CW-OSL curves, and the temperature dependence of the photoionization cross-section for the various components can be clearly discerned.     

How to visualize quartz OSL signal components

The optically stimulated luminescence (OSL) signal of natural quartz measured under constant stimulation power (CW-OSL) is a featureless decay curve where underlying components cannot be identified easily. Visual interpretation of quartz OSL signals is easier if signals are shown in spectrum-like form. This can be achieved either through ramped stimulation, or by transforming a measured CW-OSL curve into a pseudo OSL curve. We show that both give similar results, but that transformation should be preferred as CW-OSL provides best signal-to-noise ratios. We present different transformation methods to obtain pseudo OSL curves and discuss the advantages and disadvantages of each method. In addition, we show that different pseudo OSL transformations can be used to emphasize specific aspects of the OSL signal. We conclude that transformation of CW-OSL to pseudo hyperbolically modulated OSL provides the most useful visualization of the quartz fast OSL component. Pseudo parabolic modulated OSL is the transformation of choice for showing the slow component(s). The pseudo OSL curves can be used for rapid visual inspection of the relative contribution of the OSL components prior to further analysis.     

Application of the single-aliquot regenerative-dose protocol to the 375°C quartz TL signal

We report on investigations into the suitability of a single-aliquot regenerative-dose (SAR) protocol applied to the isothermal TL signal obtained from quartz held at 330°C. Samples are first thermally and optically pretreated to remove any signal from the 325°C TL trap. It is shown that the regenerated TL decay curve has the same shape as the natural one, and that recuperation is negligible. Examination of the TL glow curve before and after isothermal measurement suggests that the isothermal signal comes mainly from the 375°C TL peak, and a pulse anneal experiment is used to confirm this. This signal is bleached by simulated sunlight, with a fast component (making up about 60% of the total natural signal) bleaching about 30 times faster than a slower component. The SAR protocol is then applied to 9 samples from various depositional environments, and it is shown that the resulting data satisfy the internal checks of reliability, i.e., independence of prior treatment, and absence of recuperation. Examination of the sensitivity-corrected growth curve shows that the applicable age range for this signal may be only slightly greater than that from the OSL signal derived from the 325°C peak. This limited advantage is offset by the much greater difficulty of bleaching.     

Experimental demonstration of the variable energy of stimulation optically stimulated luminescence (VES-OSL) method

A new method of OSL stimulation using the continuous increase of stimulation energy (VES-OSL) has been previously suggested. Earlier computer simulations showed that this type of stimulation results in a peak-shaped OSL curve that closely resembles the TL peak. VES-OSL measurements were performed using a stimulation source that was specially constructed for this purpose, and the equipment is described in detail. The first results of these measurements are presented for quartz samples and the behaviour of the VES-OSL curves obtained is consistent with earlier theoretical expectations.     

The fast ratio: A rapid measure for testing the dominance of the fast component in the initial OSL signal from quartz

The signal from the fast component is usually considered preferable for quartz optically stimulated luminescence (OSL) dating, however its presence in a continuous wave (CW) OSL signal is often assumed, rather than verified. This paper presents an objective measure (termed the fast ratio) for testing the dominance of the fast component in the initial part of a quartz OSL signal. The ratio is based upon the photo ionisation cross-sections of the fast and medium components and the power of the measurement equipment used to record the OSL signal, and it compares parts of the OSL signal selected to represent the fast and medium components. The ability of the fast ratio to distinguish between samples whose CW-OSL signal is dominated by the fast and non-fast components is demonstrated by comparing the fast ratio with the contribution of the fast component calculated from curve deconvolution of measured OSL signals and from simulated data. The ratio offers a rapid method for screening a large number of OSL signals obtained for individual equivalent dose estimates, it can be calculated and applied as easily as other routine screening methods, and is transferrable between different aliquots, samples and measurement equipment.     

α-Al2O3单晶的热释光和光释光特性

研究了纯α-Al₂O₃单晶的热释光发光曲线和三维发光谱，以及光释光衰变曲线，对它们的发光机理和剂量学特性进行了分析和讨论.实验观察到α-Al₂O₃单晶β射线照射后立即测量的热释光发光曲线，有峰温为76℃和207℃两个发光峰.经γ射线照射数小时后测量的三维发光谱，只有峰温207℃波长为416 nm发光峰，它与α-Al₂O₃:C晶体的发光波长基本相同，是受热激发到导带的电子与F< 关键词： 2O₃')" href="#">α-Al₂O₃ 三维发光谱 TL/OSL剂量响应     

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.     

An improved experimental procedure of separating a composite thermoluminescence glow curve into its components

We present an improved experimental procedure of separating a composite thermoluminescence glow curve into its components. Careful monitoring of the isothermal cleaning process using the initial rise method ensures the complete thermal removal of TL peaks. Digital subtraction of two experimental TL glow curves yields individual experimental TL glow peaks. Several standard methods (initial rise and whole glow curve) are used to obtain the energy values and frequency factors of the traps. The method has been used successfully to analyze the well-known composite TL glow curve of the dosimetric material LiF (TLD-100). The limitations of the method are illustrated by analyzing the highly complex TL glow curve of a UV irradiated synthetic calcite consisting of at least 6 TL peaks. Although the method works best for TL glow curves described by first order kinetics, it should also be applicable to more general kinetics.     

Assessment of diagnostic tests for evaluating the reliability of SAR De values from polymineral and quartz fine grains

In this study, we applied optically stimulated luminescence (OSL) dating to two fine grain sediment samples collected at Jeongokri, Korea. A single aliquot regenerative dose (SAR) procedure was applied to both polymineral grains and to chemically isolated (H₂SiF₆) quartz grains of 4–11 μm diameter. For polymineral fine grains, the OSL IR depletion ratio and the equivalent dose (D_e) plateau test appear to be equally sensitive indicators of appropriate IR stimulation time for use in the ‘double SAR’ protocol. Additionally, the OSL IR depletion ratio test gives an indication of the relative mineral composition of the samples, hence providing an assessment of the likelihood of obtaining a quartz-dominated [post-IR] OSL signal. Use of higher preheat temperatures would assist in thermally eroding the non-quartz component of the [post-IR] OSL signal from polyminerals. For the quartz fine grains, data from both natural D_e determinations and laboratory dose recovery tests are required to identify the appropriate preheat temperatures for dating, due to problems of thermal transfer. This phenomenon is particularly exaggerated for these samples due to the large D_e values (≥350 Gy) and hence low slope of the dose–response curve. The double SAR method cannot be applied ubiquitously, even after careful and rigorous study of one sample from a section. Quartz OSL dating using a range of preheat temperatures is suggested to be the most suitable method for OSL dating of fine grain sediments.