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.     

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.     

Time-resolved OSL studies of YAlO3:Mn2+ crystals

Time-Resolved Optically Stimulated Luminescence (TR-OSL) from single crystalline YAlO₃:Mn²⁺ samples was investigated using a green light emitting diode (λ ∼ 525 nm) as stimulation light source. The TR-OSL decay curve of the material can be described with a single exponential decay function with a lifetime about 80 ms that does not depend on irradiation dose in the range from 50 mGy to 1 kGy. This OSL decay is superposed on a photoluminescence signal with a much shorter (3.5 ms) decay lifetime. The Mn²⁺ photoluminescence decay with a lifetime of 3.5 ms can be easily eliminated by corresponding time resolution using pulsed OSL readout. Dose response and thermal stability of the OSL signal are consistent with the previous thermoluminescent (TL) studies of the material.     

Modelling the thermal quenching mechanism in quartz based on time-resolved optically stimulated luminescence

This paper presents a new numerical model for thermal quenching in quartz, based on the previously suggested Mott-Seitz mechanism. In the model electrons from a dosimetric trap are raised by optical or thermal stimulation into the conduction band, followed by an electronic transition from the conduction band into an excited state of the recombination center. Subsequently electrons in this excited state undergo either a direct radiative transition into a recombination center, or a competing thermally assisted non-radiative process into the ground state of the recombination center. As the temperature of the sample is increased, more electrons are removed from the excited state via the non-radiative pathway. This reduction in the number of available electrons leads to both a decrease of the intensity of the luminescence signal and to a simultaneous decrease of the luminescence lifetime. Several simulations are carried out of time-resolved optically stimulated luminescence (TR-OSL) experiments, in which the temperature dependence of luminescence lifetimes in quartz is studied as a function of the stimulation temperature. Good quantitative agreement is found between the simulation results and new experimental data obtained using a single-aliquot procedure on a sedimentary quartz sample.     

More on the TR-OSL signal from BeO ceramics

Time Resolved Optically Stimulated Luminescence (TR-OSL) from BeO ceramics was investigated using blue (445 nm) and near-IR light (852 nm) for stimulation. Stimulation spectrum of the TR-OSL signal – as measured in the interval 700 to 420 nm- was observed to increase monotonically with the decreasing stimulation wavelength. In addition to the “fast” and “slow” components observed with blue light stimulation, IR stimulated TR-OSL spectra of irradiated BeO ceramics were observed to have two components with average lifetimes around ∼2.5 μs and ∼17 μs. Emission spectra of the both IR stimulated TR-OSL components were observed to have a broad emission band peaking around 330 nm. Thermal stability of the IR stimulated TR-OSL signal was studied by making preheating experiments in the range from 100 °C to 190 °C. It was observed that the IR stimulated OSL signal is stable up to ∼150 °C and decay afterwards. Radiation dose response of the IR stimulated luminescence signal was obtained in the range from 5 to 500 Gy. Both blue and IR stimulated TR-OSL signals grew up to 100 Gy and exhibited saturation for higher doses. Additionally, measurement temperature dependence of the components was also investigated and for the ∼2 μs component thermal assistance with activation energy around 0.16 eV was observed. It seems that the fast component of the blue stimulated TR-OSL component can be correlated to the ∼2 μs IR stimulated TR-OSL component.     

OSL, RL and TL characterization of rare-earth ion doped K2YF5: Application in dosimetry

Optically stimulated luminescence (OSL) properties of K₂YF₅ crystals singly doped with different concentrations of Tb³⁺ ions and doubly doped with Tb³⁺ and Ce³⁺ or Tb³⁺ and Dy³⁺ have been investigated for the first time. Radioluminescence spectra and OSL efficiency for stimulation with different wavelengths of light have been analyzed for each compound. Also, dosimetric characteristics of the most efficient composition, namely K₂YF₅:1 at.% Tb³⁺, have been studied. Finally, the OSL signal peculiarities for K₂YF₅:1 at.% Tb³⁺ have been compared to those of a commercial Al₂O₃:C dosimeter.     

Investigation of regeneration effect of blue luminescence in NaCl using variable delay optically stimulated luminescence (VD-OSL)

Optically stimulated luminescence (OSL) of pure analytical sodium chloride (NaCl) was studied. Performing series of CW-OSL (continuous wave OSL) readouts it was found that subsequent CW-OSL decay, after some delay, starts from significantly higher intensity level than the final intensity of the previous readout. To study this ‘regeneration effect’ a new type of measurements was implemented – the variable delay OSL (VD-OSL) method. The idea of VD-OSL is explained – it allows to study OSL kinetics at very long time scale. VD-OSL data confirm coexistence of two effects in NaCl – regeneration and fading of the OSL signal. After partial CW-OSL readout, regeneration predominates in the short time scale of the order of 10³ s. Then, fading becomes dominant. The same measurements were applied to commonly used Al₂O₃:C material as well. Nevertheless, the results do not show such behavior at the studied time scale. Theoretical arguments are presented that the regeneration mechanism cannot be explained on the basis of the simple trap model.     

Radiation dose response correlation between thermoluminescence and optically stimulated luminescence in quartz

The fast, linearly modulated optically stimulated luminescence (LM-OSL) component in quartz is the main dosimetric signal used for the dating applications of this material. Since the blue light stimulation (470 nm, 40 mW cm ${}^{?2}$) time needed to obtain the fast LM-OSL component is less than 50 s the electron trapping levels responsible for it are still highly populated. In this way an active radiation history is created which could play an important role in the dosimetric characteristics of the fast OSL signal. In the present work the dose response behavior of the fast OSL signal is investigated in quartz samples with an annealed radiation history and quartz samples possessing an artificial radiation history. A computerized curve de-convolution analysis of the LM-OSL curves for 50 s stimulation time showed that it consists of three individual OSL components. The faster component C₁ with peak maximum time around 5 s has a linear dose response in virgin samples, which turns to a slight superlinearity as a function of the artificial radiation history. On the other hand the component C₂ with peak maximum time at 12 s is slightly superlinear which turns into strong superlinearity as a function of artificial radiation history. Finally, component C₃ with peak maximum time at about 45 s is strongly superlinear for both virgin samples and as a function of artificial radiation history. The implications to practical application are discussed.     

The dependence of quartz OSL on stimulation energy

Quartz is the mineral most commonly used for sediment dating. In dating practice, the optically stimulated luminescence (OSL) of quartz is measured mainly using the stimulation light whose wavelength is 470 ± 30 nm. The parameters of traps active in the OSL process are also determined for this stimulation band. The zeroing of the OSL is the fundamental condition of applicability of the luminescence dating for specific sediment and takes place in sunlight whose spectrum differs significantly from the band 470 ± 30 nm. In order to be able to know the course of OSL process in nature, a wider knowledge of the dependency of the trap parameters on the stimulation band is needed. Here the results are presented for the OSL measurements carried out with different wavelengths of stimulation light. For each stimulation band the components of the OSL signal are determined by the fitting procedure, and in this way the wavelength dependence of an individual component is found. The experiment has been repeated for two temperatures of OSL detection – the room temperature, which corresponds to natural conditions, and for 125 °C, which is the temperature usually applied for OSL measurement in dating. Four OSL components are presented in both experimental series. The values of their optical cross-section changes along with stimulation energy and temperature, as it is predicted by the model of OSL process including crystal lattice vibrations.     

Assessing the impact of IR stimulation at increasing temperatures to the OSL signal of contaminated quartz

The purpose of the present study is to identify the effect of the increasing temperature IR stimulation to the component-resolved OSL luminescence signal of mixed quartz-feldspars material. Post IR OSL signals measured at 110 °C were analysed via only general order kinetic terms, while IR signals obtained at increasing temperatures were de-convolved using the sum of general order kinetics plus a tunnelling component. By increasing stimulation temperature, it was demonstrated that IRSL at temperatures above 50 °C does not only stimulate feldspar but also stimulates both fast and medium quartz OSL components. In the temperature range between 175 and 250 °C, the IRSL initial intensity is dominated by the fast OSL component. Estimated equivalent doses using either Post-IR₁₇₅.OSL₁₁₀ as well as IRSL₁₇₅ (with the indices indicating the measurement temperature) are in good agreement between each other, due to both stimulating quartz. Finally, the physical meaningfulness of the fitting parameters for the tunnelling component is also discussed.     

The TL and room temperature OSL properties of the glow peak at 110 °C in natural milky quartz: A case study

The LM–OSL signal of quartz, while measured at room temperature, is dominated by an intermediate, broad and intense OSL component, so that its contribution and general characteristics are derived very accurately. Through a series of dose–response, bleaching and thermal decay at room temperature experiments, in conjunction with curve fitting studies, a component resolved analysis is carried out studying the correlation between this specific component, termed as LM–OSL component C₂ and the 110 °C TL glow peak in quartz. The dose–response of these two luminescence components behaves exactly similar being linear at low doses and saturating at almost 100 Gy. Both signals decay exponentially under illumination, providing identical optical detrapping cross-section values. Residual of both luminescence signals after thermal decay at room temperature follows an exponential law, yielding similar mean half-lives. All previous luminescence features provide strong evidence for the electron trap being the same for both the 110 °C TL trap and the LM–OSL component C₂. The results of the present work are very promising and clearly support the possibility of extrapolating the TL pre-dose methodology to the OSL pre-dose effect using only the LM–OSL component C₂.     

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.     

Time-resolved OSL of natural zircon: A preliminary study

Time-resolved OSL (TR-OSL) from natural zircon (ZrSiO₄) minerals was investigated using 445 nm blue laser light for stimulation. Analyses of the TR-OSL spectra have showed that the decay is composed of two exponential components with lifetimes varying around ∼17 μs and around ∼110 μs respectively. The behaviour of these signal components, was examined under various sample treatments and experimental conditions. Preheating experiments showed that the OSL signal is stable up to temperatures ∼250 °C then becomes unstable. The dose response of the TR-OSL signal from zircon was determined in the range from 1 Gy to 1 kGy and observed to be increasing linearly. Practically, no effect of radiation dose on the lifetimes of signal components was observed. In addition, the effect of measurement temperature on the TR-OSL decay lifetimes was also investigated. Thermal quenching energies of the “fast” and the “slow” components were found to be very close to each other i.e. 0.18 and 0.24 eV respectively.     

Retrospective dosimetry using Japanese brick quartz: A way forward despite an unstable fast decaying OSL signal

Quartz extracted from heated bricks has been previously suggested for use in dose estimation in accident dosimetry, but this technique has never been applied before to Japanese quartz which often has unusual OSL characteristics. In this study the optically stimulated luminescence (OSL) characteristics of quartz extracted from a Japanese commercial red brick produced by Mishima – Renga – Seizoujyo Co. are studied. These companies are based in the Aichi Prefecture (capital Nagoya), which accounts for about half of the red brick production in Japan. A comparison of TL (thermoluminescence) and OSL signals has been carried out towards identification of common source traps. It is observed that OSL from Japanese brick quartz shows unusual luminescence characteristics; in particular, the initial fast decaying OSL signal contains a dominant (>90%) thermally unstable component related to the 85 °C TL peak, which necessitates a prior heat treatment. A single-aliquot regenerative-dose (SAR) protocol is developed and tested using thermal treatments intended to isolate a stable dosimetric signal. A minimum detection limit of ～65 mGy is then estimated using this protocol. Following irradiation using ⁶⁰Co and ¹³⁷Cs, dose–depth profiles were measured on two different commercial brick types (Mishima – Renga – Seizoujyo Co. and Hase – Renga Co.) with 5 Gy and 10 Gy surface doses. The profiles derived from the two sources were readily distinguishable. It is concluded that the OSL signals from the two types of Japanese brick quartz examined here can be used to derive precise estimates of accident dose, and, possibly to distinguish between sources of gamma radiation in a nuclear accident.To our knowledge, this is the first report on the existence of an unstable fast decaying OSL signal in quartz derived from bricks, and demonstrates a way forward with such samples in retrospective dosimetry.     

Use of Secondary Phosphorescence for Determining an Absorbed Dose in Dosimetric Luminophors

We consider the method of measuring optically stimulated persistence for radiation dosimetry based on separation in time of stimulating irradiation and of the recording of luminescence response. It is shown that here stimulation by shortwave radiation is possible, which is overlapped in the spectrum with the dosimetric luminophor radiation. We have measured the spectra of stimulation of a number of industrial dosimetric luminophors. The special features of the recording of optically stimulated persistence are discussed for the luminophors that contain manganese (Mn²⁺) as an activator and for which the time of decay of the luminescence which is excited within the centers is 40–50 msec. The method is applicable to the dosimetry of natural varieties of quartz for dating corresponding deposits.     

White light-emitting diodes for optical stimulation of aluminium oxide in OSL dosimetry

The results of comparative investigations into the optically stimulated luminescence (OSL) of anion-defective corundum excited by radiation of blue and white light-emitting diodes (LEDs) are reported. The continuous-wave OSL (CW-OSL) measurements showed that the white LED (compared to the blue LED) and the chosen geometry allow the amplitude of the OSL response to increase by a factor of more than 40 and the dosimetric information readout time to decrease by a factor of 20.The effect of deep traps on the behavior of the CW-OSL curves of anion-defective corundum was studied. It was found that the filling of deep traps essentially increases the TL yield with a dosimetric peak at 450 K and the CW-OSL-yield under stimulation with blue and white LEDs. It was also found that this filling causes a considerable change in the shape of the OSL curve and the time parameters of the decay.     

The estimation of basic experimental parameters in the fine-grained quartz multiple-aliquot regenerative-dose OSL dating of Chinese loess

The sensitivity-corrected multiple-aliquot regenerative-dose (MAR) protocol provides a reliable approach for fine-grained quartz optically stimulated luminescence (OSL) dating. For reliable estimation of the equivalent dose (D_e), we investigated certain basic experimental parameters in the fine-grained quartz MAR OSL dating of Chinese loess. (1) For suitable bleaching of the natural OSL signal of the regenerative-dose aliquots, the effect of bleaching duration using sunlight, SOL2 and blue LEDs on D_e was studied, and it is found that the appropriate method is a short-duration SOL2 (e.g. 5 min) or blue LEDs (e.g. 60 s) bleaching. (2) To select the appropriate test dose, the relationship between the test dose and D_e was investigated based on three samples having D_e values of approximately 11, 31 and 137 Gy respectively. It is suggested that the test dose for sensitivity correction may be limited to less than approximately 10–20 Gy. (3) Three commonly used fitting modes for quartz OSL growth curve were compared at three regenerative-dose scales. The results indicate that the mode of two saturating exponential functions plus a constant is appropriate and universal. (4) The comparison of D_e values derived using OSL approach with those obtained using the recuperated OSL (ReOSL) protocol shows that the reliable D_e estimation in the fine-grained quartz MAR OSL dating of Chinese loess may be limited to less than approximately 300 Gy. (5) The comparison of growth curves for 18 samples from the Weinan, Xifeng and Jingyuan sites shows that it is feasible to construct a standardized growth curve (SGC) for fine-grained quartz OSL signal in the Chinese Loess Plateau (CLP).     

Investigations of OSL properties of LiMgPO4:Tb,B based dosimeters

Lithium magnesium phosphate LiMgPO₄ (LMP) doped with Tb and B is one of new materials intended for use in optically stimulated luminescence (OSL) dosimetry. LMP doped with Tb and B luminophors were synthetized at IFJ PAN in Krakow. The investigations were carried out on self-developed dosimeters consisting of a slide with four LMP detectors and a light tight cover. LMP detectors were investigated in regard to their OSL properties using OSL reader named HELIOS adopted to the readouts of dosimetric cards. New LMP detectors showed high sensitivity to the ionizing radiation, good repeatability of OSL signal and good dose response, 25% of fading in the first two weeks after irradiation. Also, the pronounced dependence of OSL response on the energy of the measured radiation requires to apply the compensation filters.