Investigations into the reliability of SAR-OSL equivalent doses obtained for quartz samples displaying dose response curves with more than one component

Fast component dominated quartz single aliquot regenerative dose optically stimulated luminescence (SAR-OSL) dose response curves that display continuing growth at high doses are increasingly reported in literature. This behaviour would result in higher equivalent doses being obtained. Here we document the characteristics of OSL signals from fine (4–11 μm) and coarse (63–90 μm) quartz extracted from Romanian loess that display such behaviour. For very high doses (>1 kGy up to 5–15 kGy) the data could be closely fitted to a double saturating exponential regression model. Nonetheless, the saturation charcteristics of these fine and coarse quartz grains are very different, with average saturation chracteristic doses of D₀₁ ≈ 175 Gy and D₀₂ ≈ 1800 Gy in the case of the fine material, while in the case of the coarse material values of D₀₁ ≈ 55 Gy and D₀₂ ≈ 600 Gy have been obtained. Our results imply a hitherto unexplained mechanism in OSL production at high doses and question the reliability of obtaining SAR-OSL equivalent doses in the high dose region when a second function is needed to describe the dose response.     

Relative response of TL and component-resolved OSL to alpha and beta radiations in annealed sedimentary quartz

Knowledge of the relative luminescence response to alpha and beta radiation is very important in TL and OSL dating. In the present study the relative alpha to beta response is studied in a sedimentary quartz sample, previously fired at 900 °C for 1 h, in the dose region between 1 and 128 Gy, for both thermoluminescence (TL) and linearly modulated optically stimulated luminescence (LM – OSL). The LM – OSL measurements were performed at room temperature and at 125 °C. All OSL signals were deconvolved into their individual components. Comparison of OSL curves after alpha and beta irradiation strongly supports that quartz OSL components follow first order kinetics in both cases. In the case of TL, the relative alpha to beta response is found to be very different for each TL glow-peak, but it does not depend strongly on irradiation dose. In the case of LM – OSL measurements, it is found that the relative behaviour of the alpha to beta response is different for three distinct regions, namely the fast OSL component, the region of medium OSL component originating from the TL glow-peak at 110 °C when stimulation takes place at room temperature and finally the region of slow OSL component. Following stimulation at ambient temperature, the relative alpha to beta response of all components was not observed to depend significantly on dose, with the value of ratio being 0.03 and a tendency to decrease with increasing dose. However, in the case of measurements performed at 125 °C, the relative response of the fast components is much enhanced, and for the remaining components it increases with increasing dose. Special care must be taken to examine the relative alpha to beta response of the fast component at 125 °C which contrasts the relative response of the TL peak at ca. 325 °C. The implications for the dating of annealed quartz are also briefly discussed.     

Natural and laboratory TT-OSL dose response curves: Testing the lifetime of the TT-OSL signal in nature

This study compares natural and laboratory generated thermally transferred optically stimulated luminescence (TT-OSL) dose response curves (DRCs) for fine-grain quartz extracts from the Luochuan loess section in central China. Both DRCs saturate at high doses relative to the quartz OSL signal; the natural TT-OSL DRC saturates at about 2200 Gy and laboratory DRCs saturate at about 2700 Gy. However, the natural and laboratory TT-OSL DRCs deviate from one another at circa 150 Gy resulting in TT-OSL equivalent dose underestimation relative to palaeodoses expected from dose rates and independent age control. The lifetime of the TT-OSL signal at 10 °C, calculated from values of trap parameters E and s, is compared against the value for lifetime of the TT-OSL signal in nature at average burial temperature as determined from the age underestimation caused by deviation of the natural and laboratory generated DRCs. These two independent assessments of TT-OSL signal lifetime at Luochuan give similar values, suggesting that laboratory measurements of thermal stability reflect natural burial lifetimes and can potentially be used to correct TT-OSL ages for the difference between natural and laboratory dose response curves.     

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).     

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.     

TL and OSL dosimetric properties of Opal gemstone for gamma radiation dosimetry

In this work, the response of the natural material Opal was studied in relation to its thermoluminescence (TL) and optically stimulated luminescence (OSL), after exposure to the gamma radiation of a ⁶⁰Co source. The structure of the powdered Opal was verified using the X-ray diffraction, scanning electronic microscopy and energy-dispersive X-ray spectroscopy techniques. The material, in its stone form, was turned into powder and mixed to Teflon (also in powder) in three different concentrations, and then pellets were manufactured. The aim of this work was to evaluate the response of these pellets in high-doses of gamma radiation beams, and to observe their possible application as dosimeters, using the TL and OSL techniques. The dosimetric properties of the samples were analyzed by means of different tests, as: TL emission curves and OSL signal decay curves, reproducibility of TL and OSL response, minimum detectable dose, TL and OSL dose–response curves (5 Gy–10 kGy), and fading. The results obtained in this work, for the TL and OSL phenomena, demonstrated that the pellets of Opal + Teflon present an adequate performance e possibility of use as dosimeters in beams of high-dose gamma radiation.     

Study of the luminescent behavior of Spectrolite + Teflon pellets in 90Sr + 90Y beams

The Spectrolite, from the silicate family, a variety of Labradorite, was already studied in relation to its thermoluminescence (TL) and optically stimulated luminescence (OSL) responses, in high-dose gamma radiation fields; the results indicated their good application as gamma radiation detectors. In the present work, the analyses performed to investigate powdered Spectrolite are presented, by means of the XRD, SEM and EDX techniques. The luminescent behavior of Spectrolite + Teflon samples, in the concentration of 1:1, was studied in beta radiation beams (⁹⁰Sr + ⁹⁰Y), using the luminescent phenomena of TL and OSL. The results showed adequate TL and OSL reproducibility of the samples; the dose–response curves for both techniques presented a linear behavior in a range from 0.5 Gy to 1 kGy, and the fading showed that after 150 h there were 46.7% and 31.6% of the remaining signal of samples for TL and OSL responses, respectively. Therefore, the Spectrolite + Teflon pellets may be used in beta radiation dosimetry.     

A comparison of single and multiple aliquot TT-OSL data sets for sand-sized quartz from the Arabian Peninsula

The quartz OSL signal from dune sands from Saudi Arabia and Oman start to saturate at doses of about 100 Gy. In order to try to date dune sands with greater expected doses, a previously published, single-aliquot, regenerative-dose protocol (SAR) for thermally-transferred optically stimulated luminescence (TT-OSL) was tested. Dose recovery tests, recycling and recuperation ratios showed robust functioning and dose response curves demonstrated the potential to extend the dose range to beyond 600 Gy. Multiple aliquot additive dose (MAAD) TT-OSL protocols were used to test for sensitivity changes in the SAR TT-OSL protocol up to doses of 1200 Gy. A strong dose dependent deviation of the SAR TT-OSL relative to the MAAD TT-OSL dose response is observed. Comparison of the TT-OSL and OSL sensitivity data obtained from the MAAD and SAR data sets shows a lack of proportionality between TT-OSL and OSL for the SAR data which will result in a problem when SAR dose response curves are constructed using many regeneration points with doses above 300 Gy.     

Investigating quartz optically stimulated luminescence dose–response curves at high doses

Despite the general expectation that optically stimulated luminescence (OSL) growth should be described by a simple saturating exponential function, an additional high dose component is often reported in the dose response of quartz. Although often reported as linear, it appears that this response is the early expression of a second saturating exponential. While some studies using equivalent doses that fall in this high dose region have produced ages that correlate well with independent dating, others report that it results in unreliable age determinations. Two fine grain sedimentary quartz samples that display such a response were used to investigate the origin of this additional high dose component: three experiments were conducted to examine their dose–response up to >1000 Gy. The high dose rates provided by laboratory irradiation were found not to induce a sensitivity change in the response to a subsequent test dose, with the latter not being significantly different from those generated following naturally acquired doses. The relative percentage contributions of the fast and medium OSL components remained fixed throughout the dose–response curve, suggesting that the electron traps that give rise to the initial OSL do not change with dose. An attempt was made to investigate a change in luminescence centre recombination probability by monitoring the depletion of the ‘325 °C’ thermoluminescence (TL) during the optical stimulation that would result in depletion of the OSL signal. The emissions measured through both the conventional ultraviolet (UV), and a longer wavelength violet/blue (VB) window, displayed similar relative growth with dose, although it was not possible to resolve the origin of the VB emissions. No evidence was found to indicate whether the additional component at high doses occurs naturally or is a product of laboratory treatment. However, it appears that these samples display an increased sensitivity of quartz OSL to high doses that is not recorded by the sensitivity to a subsequent test dose, and which results in a change in the sensitivity-corrected dose–response curve.     

Cross-calibration between beta and gamma sources using quartz OSL: Consequences of the use of the SAR protocol in optical dating

The radiation dose delivered by the ⁹⁰Sr beta source of a TL-OSL reader and the one delivered by a ¹³⁷Cs gamma source were compared using OSL dating techniques and tools. Three sets of quartz of different origins (rock, sediment and loess) were studied and measured by the SAR protocol (Single aliquot regenerative dose protocol) after irradiations carried out either by the ⁹⁰Sr source or by a ¹³⁷Cs source. Measurements show that the values obtained by the SAR protocol must be corrected in order to provide an acceptable cross-calibration of the beta and gamma source. Once applied, measurement sets become self-consistent and compatible with expected values. The consequences of the above mentioned observations on the methodology of OSL dating are discussed and suggest that a mixed protocol be used including both the SAR protocol and an added dose techniques close to the SARA protocol (Single aliquot regenerative and added dose protocol).     

A comparison of natural- and laboratory-generated dose response curves for quartz optically stimulated luminescence signals from Chinese Loess

It has previously been observed that laboratory-generated quartz optically stimulated luminescence (OSL) signals from different samples have similar dose response curves (DRCs) after they are normalized using a test dose. It therefore seems likely that growth of the normalized signal due to natural irradiation of quartz may also follow a general dose response curve. The existence of such a curve is investigated by constructing a natural DRC from the test dose-normalized natural OSL signals of seven samples from the Luochuan section of the Chinese Loess Plateau. The same aliquots are then used to build single aliquot regenerative (SAR) DRCs, making it possible to compare the natural and laboratory constructed curves. Two main differences are observed. Firstly, the laboratory-generated DRCs are best fitted with double saturating exponential functions whereas the natural DRC is equally well fitted with a single saturating function. Secondly, in the laboratory-generated DRCs the normalized OSL signal continues to increase at high laboratory doses (>500 Gy), whereas no growth is seen at these doses in the equivalent natural DRC. These differences between natural- and laboratory-generated DRCs are still apparent even if data are manipulated to isolate the fast component, or if a sensitivity corrected multiple aliquot regenerative (SC-MAR) dose procedure is used. This suggests that the observed differences are not due to the influence of different components or inter-regenerative dose cycle sensitivity changes. The divergence between the natural- and laboratory-generated DRC means that the current maximum limit of quartz OSL dating at the Luochuan section is 150 Gy, as D_e estimates above this value are likely to be underestimations.     

Using optically stimulated electrons from quartz for the estimation of natural doses

A flow-through Geiger-Müller pancake electron detector attachment has been fitted to a standard Risø TL/OSL reader enabling optically stimulated electrons (OSE) to be measured simultaneously with optically stimulated luminescence (OSL). Using this detector, OSE and OSL measurements from natural quartz samples are studied to examine the possible use of OSE as a chronometer. First the relative variability in OSE and OSL growth curve shapes and the effect of preheat on these are presented, and from these curves, conclusions are drawn concerning the charge movement in natural quartz. Secondly, a dose recovery test shows that OSE can successfully recover a laboratory dose of 300 Gy given before any laboratory thermal treatment, for preheating temperatures between 160 and 260 °C. Furthermore, for the first time natural OSE decay curves are detected and these signals are used to estimate a burial dose using the single-aliquot regenerative-dose (SAR) procedure. Finally, a comparative study of the equivalent doses estimated using both OSE and OSL from 10 quartz samples are presented, and it is shown that OSE has a significant potential in retrospective dosimetry.     

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.     

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.     

A new irradiated quartz for beta source calibration

For luminescence dating to be an accurate absolute dating technique it is very important that we are able to deliver absolutely known radiation doses in the laboratory. This is normally done using a radiation source (alpha, beta, X-ray) calibrated against an absolutely known reference source. Many laboratories have used the various different batches of Risø calibration quartz for the calibration of beta and X-ray sources, but these have been largely undescribed. Here we describe in detail the preparation and luminescence characteristics of a new quartz standard, based on a North Sea beach sand collected from south-western Denmark (Rømø). Two grain sizes (4–11 μm and 180–250 μm) have been examined in detail. These were pre-treated (annealed, dosed and annealed again) to sensitise and stabilise the luminescence signals before being given an absolutely known gamma dose from a point ¹³⁷Cs source in scatter-free geometry. The luminescence characteristics are described; the very intense blue-light stimulated signal is dominated by the fast OSL component and the IR-stimulated signal is negligible. The material is shown to be suitable for measurement using SAR, and the dose recovery ratio is indistinguishable from unity with a standard deviation of <2% for multi-grain aliquots. The material is also shown to be suitable for single-grain calibration, with >80% of the grains giving a useful signal. Although there is an unexplained dispersion in our calibration data of ∼3% (which we cannot attribute to instrument variability), we nevertheless conclude that this material is very suitable for transferring absolute known doses from a standardised gamma source to in-built irradiation sources.     

Distinguishing dose populations in sediment mixtures: a test of single-grain optical dating procedures using mixtures of laboratory-dosed quartz

Many natural deposits contain grains that have different burial histories, but reliable procedures to extract the component doses from mixed-dose samples have not been developed in optical dating. Here we present results for synthetic two- and three-component mixtures of data derived from laboratory-dosed sedimentary quartz using a single-aliquot regenerative-dose protocol and statistical models for finite mixtures. Composite sets of data were created from the doses measured for individual grains that had been bleached by sunlight and then given a beta dose of 5, 10 or 20 Gy. We found that the correct number of dose components, corresponding doses, and relative proportions of each component may be estimated if the within-component dispersion is small or is known. We also found, however, that recuperation of the OSL signal in sun-bleached quartz may produce artificially high dose estimates for some grains, an effect that should be taken into account when modelling natural mixtures.     

Optically stimulated luminescence from BeO ceramics: An LM-OSL study

Optically Stimulated Luminescence (OSL) signals of BeO ceramics were investigated using continuous wave (CW) OSL and Linearly Modulated (LM) OSL. It was found that both curves can be approximated using a linear combination of two first-order components. Experiments on the measurement temperature dependence have shown that these two components have nearly the same thermal quenching energies around 0.57 eV. Dependences of the OSL signal on preheat temperature and radiation dose were also examined. Thermal annealing experiments have shown that OSL signals originate from traps which are unstable near 340 °C, thus proving the suitability of the signals for dosimetric purposes. Dose response was found to be linear and a minimum detectable dose of ～10 μGy was found.     

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.     

OSL and TL retrospective dosimetry with a fluorapatite glass-ceramic used for dental restorations

Optically Stimulated Luminescence (OSL) and Thermoluminescence (TL) properties of a fluorapatite glass-ceramic have been investigated, with a view to developing a dose assessment technique for medical triage following unplanned exposures of individuals to ionizing radiation. The ceramic is an innovative material used in dental prostheses and restorations. It is strongly sensitive to radiation and the intensity of both the OSL and TL signals are proportional to the absorbed radiation dose. We focused on the optimization of the measuring procedure and investigated characteristics such as reproducibility, fading, minimum detectable dose (MDD), dose response and photon energy response of TL and OSL signals. The dental ceramic exhibited very good reproducibility (<5% at 2σ level) when measured and a linear dose response for a wide range of doses (50 mGy–20 Gy). The MDD values for the samples investigated were ∼5 mGy. The material is not tissue equivalent and the OSL and TL signals are strongly dependent on incident photon energy. Both the luminescence signals exhibited significant fading during the first few hours after irradiation. Its rate was dependent on the parameters of measurement. The results indicate that the material can be used for the purposes of accident dosimetry, however, the fading and photon energy response have to be properly corrected for a reliable dose assessment.     

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.