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.     

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.     

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.     

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.     

Correlation of optically and thermally stimulated luminescence of natural fluorite pellets

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

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

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

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.     

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.     

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.     

Optically stimulated luminescence from quartz measured using the linear modulation technique

The optically stimulated luminescence (OSL) from heated natural quartz has been investigated using the linear modulation technique (LMT), in which the excitation light intensity is increased linearly during stimulation. In contrast to conventional stimulation, which usually produces a monotonically decreasing signal, linearly increasing the stimulation power gives peaks in the signal as a function of time. In cases where the OSL signal contains more than one component, the linear increase in power of the stimulation light may result in a curve containing overlapping peaks, where the most easily stimulated component occurs at a shorter time. This allows the separation of the overlapping OSL components, which are assumed to originate from different traps. The LM-OSL curve from quartz shows an initial peak followed by a broad one. Deconvolution using curve fitting has shown that the composite OSL curve from quartz can be approximated well by using a linear combination of first-order peaks. In addition to the three known components, i.e. fast, medium and slow components from continuous-wave-OSL studies, an additional slow component is also identified for the first time. The dose responses and thermal stabilities of the various components are also studied.     

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.     

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.     

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.     

The problem of dating quartz 2: Synchrotron generated X-ray excited optical luminescence (XEOL) from quartz

The luminescence emission of quartz is used in optically stimulated luminescence dating (OSL), however the precise origins of the emission are unclear. A suite of quartz samples were analysed using X-ray excited optical luminescence (XEOL). Radiation dose effects were observed whereby the UV emissions (3.8 and 3.4 eV) were depleted to the benefit of the red emission (1.9–2.0 eV). Samples were excited at ∼7 keV. Understanding why some quartz emit light more brightly than others will increase the efficiency and precision of OSL analyses.     

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.     

Ionization density dependence of the curve shape and ratio of blue to UV emissions of Al2O3:C optically stimulated luminescence detectors exposed to 6-MV photon and therapeutic proton beams

In this work we characterized the dose and linear energy transfer (LET) (ionization density) dependence of commercial Al₂O₃:C optically stimulated luminescence (OSL) detectors (OSLDs) exposed to clinical photon and proton beams. We characterized the dose-dependence of the OSL signal, OSL curve shape, and the relative intensities of the blue and ultraviolet (UV) OSL emission bands using different readout protocols and beam qualities. We irradiated OSLDs with absorbed doses ranging from 0.1 Gy to 100 Gy in a 6-MV photon beam and from 0.1 Gy to 50 Gy in 140- and 250-MeV proton beams. Readouts were done with both continuous-wave (CWOSL) and pulsed (POSL) stimulation. The linearity of the OSLD dose–response depended on readout protocol and radiation type. Improved linearity was found for OSLDs irradiated with beams of increased LET, and for OSL signals containing only the blue emission band of Al₂O₃:C (which remained linear for doses up to 10 Gy for 140-MeV proton beam irradiations). The OSL curve shape did not vary with dose in the low-dose region (below 5 Gy depending on readout protocol), but beyond this, curves decayed more rapidly with increasing dose. Similarly, the ratio of blue to UV emission band intensities in the OSL signal did not vary with dose up to 5 Gy (depending on readout protocol), beyond which the ratio decreased with increasing dose. Because both the OSL curve shape and the ratio of blue to UV emission intensities have been investigated as potential parameters for measurements of LET, the constancy of these two quantities at doses relevant to radiotherapy is encouraging for the potential development of novel OSL methods to measure LET. Our findings are expected to contribute to the development of (i) improved readout protocols for commercially available Al₂O₃:C OSLDs and (ii) methods to measure radiation quality and LET.     

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.     

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.