The response of thermally and optically stimulated luminescence from Al2O3:C to high-energy heavy charged particles

The thermoluminescence (TL) and optically stimulated luminescence (OSL) response of Al₂O₃ dosimeters to high-energy heavy charged particles (HCP) has been studied using the heavy ion medical accelarator at Chiba, Japan. The samples were Al₂O₃ single-crystal chips, of the type usually known as TLD-500, and Luxel^TM dosimeters (Al₂O₃:C powder in plastic) from Landauer Inc. The samples were exposed to ⁴He (150 MeV/u), ¹²C (400 MeV/u), ²⁸Si (490 MeV/u) and ⁵⁶Fe (500 MeV/u) ions, with linear energy transfer values covering the range from 2.26 to 189 keV/μm in water and doses from 1 to 100 mGy (to water). A ⁹⁰Sr/⁹⁰Y beta source, calibrated against a ⁶⁰Co secondary standard, was used for calibration purposes. For OSL, we used both continuous-wave OSL measurements (CW-OSL, using green light stimulation at 525 nm) and pulsed OSL measurements (POSL, using 532 nm stimulation from a Nd:YAG Q-switched laser). The efficiencies (η_HCP,γ) of the different HCPs at producing OSL or TL were observed to depend not only upon the linear energy transfer (LET) of the HCP, but also upon the sample type (single crystal chip or Luxel^TM) and the luminescence method used to define the signal—i.e. TL, CW-OSL initial intensity, CW-OSL total area, or POSL. Observed changes in shape of the decay curve lead to potential methods for extracting LET information of unknown radiation fields. A discussion of the results is given, including the potential use of OSL from Al₂O₃ in the areas of space radiation dosimetry and radiation oncology.     

Thermoluminescence and optically stimulated luminescence characteristics of Al2O3 doped with Tb

In the present work policrystals of α − Al₂O₃ doped with terbium were synthesized using the solvent evaporation method. The samples were prepared using Al(NO₃)₃·9H₂O and Tb(NO₃)₃·5H₂O reagents, with Tb concentrations between 1 and 5 mol% and thermally treated at high temperature above ∼1400 °C. X-ray diffraction measurements showed the α-phase formation of samples. TL glow curve presented an intense peak at ∼190 °C and two other with low intensity at 290 and 350 °C after gamma irradiation. The best doping concentration which presented high luminescence was the sample doped with 3 mol% of Tb. TL spectra and fluorescence measurements showed similar luminescence spectra with lines attribute to Tb³⁺ ions. A linear behavior to gamma dose between 1 and 20 Gy was observed in TL, using 190 °C peak as well as in OSL signal, this last carried out using 532 nm wavelength stimulation.     

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.     

The response of thermally and optically stimulated luminescence from Al2O3:C to high-energy heavy charged particles

The thermoluminescence (TL) and optically stimulated luminescence (OSL) response of Al₂O₃ dosimeters to high-energy heavy charged particles (HCP) has been studied using the heavy ion medical accelarator at Chiba, Japan. The samples were Al₂O₃ single-crystal chips, of the type usually known as TLD-500, and Luxel^TM dosimeters (Al₂O₃:C powder in plastic) from Landauer Inc. The samples were exposed to ⁴He (150 MeV/u), ¹²C (400 MeV/u), ²⁸Si (490 MeV/u) and ⁵⁶Fe (500 MeV/u) ions, with linear energy transfer values covering the range from 2.26 to 189 keV/μm in water and doses from 1 to 100 mGy (to water). A ⁹⁰Sr/⁹⁰Y beta source, calibrated against a ⁶⁰Co secondary standard, was used for calibration purposes. For OSL, we used both continuous-wave OSL measurements (CW-OSL, using green light stimulation at 525 nm) and pulsed OSL measurements (POSL, using 532 nm stimulation from a Nd:YAG Q-switched laser). The efficiencies (η_HCP,γ) of the different HCPs at producing OSL or TL were observed to depend not only upon the linear energy transfer (LET) of the HCP, but also upon the sample type (single crystal chip or Luxel^TM) and the luminescence method used to define the signal—i.e. TL, CW-OSL initial intensity, CW-OSL total area, or POSL. Observed changes in shape of the decay curve lead to potential methods for extracting LET information of unknown radiation fields. A discussion of the results is given, including the potential use of OSL from Al₂O₃ in the areas of space radiation dosimetry and radiation oncology.     

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.     

Response variation of optically stimulated luminescence dosimeters

This study investigates the variability in response of optically stimulated luminescence dosimeters (OSLDs). Examining the source of sensitivity variations in these dosimeters allows for a more comprehensive understanding of the Landauer nanoDots and their potential for current and future applications. In this work, OSLDs were scanned with a MicroCT scanner to determine potential sources for the variation in relative sensitivity across a selection of Landauer nanoDot dosimeters. Specifically, the correlation between a dosimeters relative sensitivity and the loading density of Al₂O₃:C powder was determined. When extrapolating the sensitive volume's radiodensity from the CT data, it was shown that there is a non-uniform distribution in crystal growth. It was calculated that a 0.05% change in the nominal volume of the chip produces a 1% change in the overall response. Additionally, the ‘true’ volume of an OSLD's sensitive material is, on average, 18% less than that which has been reported in literature, mainly due to the presence of air cavities in the material's structure. This work demonstrated that the amount of sensitive material is approximately linked to the total correction factor.     

Al2O3:C optically stimulated luminescence droplets: Characterization and applications in medical beams

Optically stimulated luminescence (OSL) detectors, which are widely used in radiation protection, offer a number of potential advantages for radiotherapy dosimetry. In this study we characterized 1-μl of OSL droplets consisting of a mixture of Al₂O₃:C powder and a photo-curable polymer, in addition to results described in a previous work (Nascimento et al., 2013). The concentration test showed that droplets have a higher spatial resolution than other commonly used Al₂O₃:C-based detectors. Our results from the dose response, reproducibility and dependence with accumulative dose were obtained for droplets with a powder/polymer concentration that showed a high Signal to Noise Ratio (SNR) without compromising the droplet malleability. Additional test results show the response of such droplets in percentage depth dose curves and dose profiles of clinical beams.     

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.     

Peculiarities of optically stimulated luminescence in halite

Sodium chloride – NaCl is one of materials indicating strong OSL signal after exposure on ionizing radiation. Previous studies of the OSL response in pure sodium chloride showed coexistence of fading and regeneration of the signal using the newly developed variable delay optically stimulated luminescence technique (VD-OSL). This paper presents investigations of some peculiarities of long time scale OSL properties of rock salt (halite) including sensitization phenomena for various bleaching methods. Dose response characteristics were studied in the range from 200 mGy to 1 Gy for series of halite aliquots without signal bleaching and for single aliquot using zeroing by blue and green light.     

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.     

A time-correlated photon counting system for measurement of pulsed optically stimulated luminescence

A versatile light-emitting-diode system for measurement of time-resolved luminescence spectra is described. The instrument is an improvement on a previously reported version [1] also based on pulsed light-emitting diodes. The present configuration offers substantially improved performance in measurement of time-resolved optically stimulated luminescence spectra and records the luminescence with better dynamic throughput. Measurements made on sedimentary quartz annealed at 800 °C as an exemplar show that the luminescence obtained after the light pulse as a proportion of the total measured signal falls within the usable dynamic range of 0.1-98% for pulse-widths between 3 and , a range of pulse-widths and so luminescence yield that is sufficient for most contemporary applications of time-resolved optically stimulated luminescence.     

Test for quasi-equilibrium in thermally stimulated luminescence and conductivity

The uncertainty about the existence of quasi-equilibrium (QE) condition during the readout of thermoluminescence and thermally stimulated conductivity glow peaks in real materials causes doubts about the validity of applying the QE-based analytical expressions to analyse these glow peaks. In this paper a simple method is given to verify the QE condition during the readout of these glow peaks in real materials. The method is based on changes in the glow peak shapes caused by changing the heating rate in non-QE cases. It is illustrated by using synthetic glow peaks derived from two different physically meaningful models.     

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.     

Estimating the parameters of traps in quartz by the variable energy of stimulation optically stimulated luminescence (VES-OSL) method

Optical-cross section that is a trap parameter estimated from the measurements of optically stimulated luminescence (OSL) is not a uniquely determined physical quantity. It depends not only on temperature and the energy of stimulation light but also, in the simplest case, on the optical depth of trap, the frequency of vibration mode and on the Huang-Rhys factor, i.e. the average number of phonons involved in the process of optical excitation of electrons from trap to conduction band. Conventional OSL measurement techniques do not enable to determine directly these parameters but they could be estimated by applying the variable energy of stimulation optically stimulated luminescence (VES-OSL) method. Recently it was put in to practice and the first VES-OSL curves were presented. In this study the outcomes of VES-OSL experiments are presented together with the first attempt of direct estimating the optical depth of traps active in OSL process in quartz.     

Behavioural studies of stimulated luminescence from feldspars

Since the work of Mejdahl in the mid-1980s feldspars have been used widely for palaeodosimetry. They have proved particularly popular because of the technical ease with which an optically stimulated luminescence signal can be obtained, and the potential for their use in dating over a wider time range than quartz. However, while the use of infrared stimulated lminescence has been a great success, the realisation of the potential for dating over a wide time range has been hampered by a series of behavioural problems, in particular concerned with the stability of the luminescence signal. This paper surveys the current state of knowledge of a range of aspects of the stimulated luminescence behaviour of feldspar. Particular attention is paid to the thermal and optical properties of the thermoluminescence (TL) and optically stimulated luminescence (OSL) signals from feldspars since these are of greatest relevance to their use as palaeodosimeters. Results obtained from well-characterised museum specimens demonstrate the variety of responses that are seen from different types of feldspar, particularly in their TL behaviour. Less variation is seen in their OSL response. In contrast, the response of potassium-rich feldspars separated from Quaternary sediments tends to be very consistent when many grains are analysed simultaneously, suggesting that averaging of the signal simplifies the behaviour of the system.     

Radiation induced luminescence processes in c-BN

Spectral properties of cubic boron nitride have been studied using methods of photoluminescence (PL), X-ray excited luminescence (XL), thermoluminescence (TL) and optically stimulated luminescence. It is found that emission of cubic boron nitride is presented by 4 subbands, their relative yield is determined by the excitation type: blue, green (dominant) and red bands are observed in PL, ultraviolet, blue (dominant), green and red bands—in XL. Three thermal peaks are found in TL curves in the 0–700°C temperature range, their presence and intensity depend on radiation type used. A tentative correspondence between thermal peaks and emission bands is found.     

Thermally and optically stimulated radiative processes in LiBaF3 crystals

In LiBaF₃ crystals both valence–core transitions (5.4–6.5 eV) and so-called self-trapped exciton luminescence (about 4.3 eV) are important for practical application. Here, we present a study of 4.3 eV luminescence under photo- and thermostimulation after X-irradiation of undoped LiBaF₃ crystals at various temperatures. Optically stimulated luminescence as a result of electron recombination with both self-trapped holes and holes localized at some defects, were observed after X-irradiation below 130 K and that of electron recombination with defect-localized holes was observed after X-irradiation above 130 K. The spectra of thermo-stimulated luminescence (TSL) contain a broad band about 4 eV related to the electron (high-energy side) or hole (low-energy side) recombination depending on TSL peak temperature.     

Optically stimulated luminescence in doped K3Na(SO4)2 phosphors

Optically stimulated luminescence (OSL) in Cu and Eu doped K₃Na(SO₄)₂ is reported for the first time. The Cu-doped sample shows OSL sensitivity which gets enhanced by co-doping with Mg²⁺ ions. The Cu-doped and quenched sample shows better sensitivity which is almost double than that of the slowly cooled sample, whereas the sensitivity of Mg co-doped sample remains nearly same irrespective of the thermal treatment. The Cu-doped sample shows TL peak around 200 °C and moderate OSL sensitivity. Doping of Mg shifts the TL peak to around 160 °C and is correlated with good OSL sensitivity. Eu-doped sample does not show OSL sensitivity. However, relatively good OSL sensitivity is observed in Aluminium co-doped and slowly cooled sample, which is about 15% of the commercial Al₂O₃:C(Landuer Inc.). A near fully optically sensitive TL peak around 155 °C is observed. The dose response is linear and practically no OSL fading is observed in first five days of storage in slowly cooled sample. This study on conventional sulphate-based TL phosphors will be useful in developing OSL phosphors for radiation dosimetry.     

Kinetics of thermally stimulated luminescence from alkaline earth borates

The kinetics of thermally stimulated emission (TSL) from XB₂O₄ (X= Ca, Sr, Ba) has been investigated employing both isothermal decay and peak shape analysis methods. For BaB₂O₄ the emission was observed to lie in the visible region and the kinetics of TSL emission could be determined without any ambiguity. However, the emission spectra of CaB₂O₄ and SrB₂O₄ were found to consist of two broad emissions: one in the UV and the other in the blue green regions. Consequent to the presence of two emission bands, the determination of TSL kinetics required collection of TSL data for the two components of emission separately. Otherwise, an unambiguous determination of the TSL kinetics just could not be possible. The kinetics of TSL emission for the three borates is found to be of second order.     

Insect wings as retrospective/accidental/forensic dosimeters: An optically stimulated luminescence investigation

Estimation of the radiation released during nuclear accidents or radiological terrorist events is imperative for the prediction of health effects following such an exposure. In addition, in several cases there is a need to identify the prior presence of radioactive materials at buildings or sites (nuclear forensics). To this direction, several materials have been the research object of numerous studies the last decade in an attempt to identify potentially new retrospective/accidental/forensic dosimeters.However, the studies targeting biological materials are limited and their majority is mainly focused on the luminescence behavior of human biological material. Consequently, the use of such materials in retrospective dosimetry presumes the exposure of humans in the radiation field. The present work constitutes the first attempt to seek non-human biological materials, which can be found in nature in abundance or in/on other living organisms. To this end, the present work investigates the basic optically stimulated luminescence behavior of insect wings, which exhibit several advantages compared to other materials. Insects are ubiquitous, have a short life expectancy and exhibit a low decomposition rate after their death.Findings of the present study are encouraging towards the potential use of insects' wings at retrospective/accidental/forensic dosimetry, since they exhibit linear OSL response over a wide dose range and imperceptible loss of signal several days after their irradiation when they are kept in dark. On the other hand, the calculated lower detection limit is not low enough to allow their use as emergency dosimeters when individuals are exposed to non-lethal doses. In addition, wings exhibit strong optical fading when they are exposed to daylight and thus special care should be taken during the sampling procedure in order to use the wings as accidental/forensic dosimeters, by seeking (dead) insects in dark places, such as behind furniture, equipment or in air-shafts.Finally, a new single aliquot measurement protocol is also successfully tested on the wings for the dose estimation, while further work is in progress to validate it on other (heat-sensitive) materials as well.