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 the thermally transferred optically stimulated luminescence source trap in fired geological quartz

The pre-dosed thermoluminescence (TL) emission of quartz has been found to be useful in retrospective dosimetry and archaeometry. Though the pre-dosed optically stimulated luminescence (OSL) and TL emissions have been reported to be similar, the former has been found to be un-reliable for the equivalent dose estimation. As this measurement protocol involves thermal heating at around 400 °C, the work reported in this paper investigated the influence of this heating on the OSL using fired specimens from various regions. The results suggested that the discrepancy in the behaviour of two emissions is caused by the presence of the thermally transferred optically stimulated luminescence (TT-OSL) induced by thermal-activation involved in the pre-dose treatment. This transferred signal was observed to be very significant in the case of samples containing a prominent higher-temperature TL peak at ∼375 °C. The characterization of this signal based on (i) the nature of the glow curves, (ii) thermal-annealing of the OSL trap, (iii) observation of the TT-OSL, (iv) bleaching of the source trap and (v) the correlation between TL and OSL seems to suggest that the trap corresponding to this TL peak is the source trap in the TT-OSL emission mechanism.     

Evaluating the efficiency of TT-OSL SAR protocols

Optically Stimulated Luminescence (OSL) dating based on the fast component is now widely used to establish chronologies of sedimentary deposits. Since this component saturates at a relatively low dose, the method is limited to the dating of Late Pleistocene quartz samples. Consequently, dating events beyond this limit is a key challenge. In this context the use of the TT-OSL signal which exhibits a high doses saturation level offers the potential to extend the age range of the method. Since the promising study of Wang et al. (2006b), in which a 780 ka age validated by palaeomagnetism data was reported for a Chinese loess sample, several studies focused on establishing a SAR TT-OSL dating protocol. They suggested applying different kinds of heat treatment at the end of a SAR cycle, as well as two normalisation procedures. The aim of this study was to test the reliability of these protocols for a loess-like Middle Pleistocene sample for which the expected De is known approximatively. We tested four published SAR protocols by implementing the dose recovery tests on artificially bleached quartz aliquots. The results obtained showed a systematic overestimation of the recovered doses and revealed high sensitivity changes between the first (natural) and the following cycles. It is believed that this behaviour is a consequence of the thermal treatment applied at the end of each SAR cycle which is necessary to empty the hard-to-bleach TT-OSL traps. Neither OSL nor TT-OSL signal test dose responses proved suitable to correct this sensitivity change.     

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.     

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.     

Dose dependence of thermally transferred optically stimulated luminescence signals in quartz

The thermally transferred optically stimulated luminescence (TT-OSL) responses of chemically purified fine-grained quartz from seven loess-like samples from Korea are presented. In particular, the experimental procedures used to separate the dose-dependent (recuperated OSL, ReOSL) and dose-independent parts of the signal were explored. The OSL signals used to monitor the sensitivity changes that take place during the measurement sequences used to determine the equivalent dose were investigated. A single aliquot procedure was used for the TT-OSL measurements and resulted in linear growth of the ReOSL with dose up to at least 2 kGy. For this suite of samples, a standardised growth curve (SGC) was constructed for the ReOSL, tested with dose recovery experiments, and was used to obtain D_e values for the seven samples.     

Study of the 110°C TL peak sensitivity in optical dating of quartz

As the 110°C TL emission in quartz uses the same luminescence centers as the OSL emission, the 110°C TL signal from a test dose may be used to monitor the OSL sensitivity change. It is thus important to study the relationship between the 110°C TL peak and the OSL sensitivity in studies related to optical dating from quartz. We have conducted a series of experiments using sedimentary quartz, where the annealing temperatures were varied between 260 and 1000°C before the measurement of OSL and 110°C TL sensitivities. Another series of experiments on two sedimentary quartz samples investigated the 110°C TL peak and OSL dose-dependent sensitivity change after different annealing temperatures. In these experiments, the 110°C TL and OSL signals from the test dose are shown to have similar sensitization characteristics: the 110°C TL sensitivity change is proportional to the OSL sensitivity change if the annealing temperature is lower than 500°C. It is concluded that the 110°C TL signal can be used to correct the OSL sensitivity change in the single-aliquot additive-dose protocol.     

Observations of thermal transfer OSL signals in glacigenic quartz

The conclusions of Rhodes and Pownall (Rhodes, E.J., Pownall, L., 1994. Zeroing of the OSL signal in quartz from young glaciofluvial sediments. Radiation Measurements 23, 329–333) were somewhat discouraging for the prospects of using quartz OSL for dating glacigenic sediments, while the more detailed study of Rhodes and Bailey (Rhodes, E.J., Bailey, R.M., 1997. The effect of thermal transfer on the zeroing of the luminescence of quartz from recent glaciofluvial sediments. Quaternary Science Reviews (Quaternary Geochronology) 16, 291–298) provided more encouragement. Specifically, the latter authors were able to account for the relatively high D_e values observed for recent glacigenic (dominantly glaciofluvial) sediments in terms of an anomalously high thermal transfer effect, rather than simply insufficient bleaching prior to deposition. In other locations, the OSL of quartz from glacigenic material appears to provide reliable age estimates, and does not suffer from these effects (Owen, L.A., Richards, B., Rhodes, E.J., Cunningham, W.D., Windley, B.F., Badamgarav, J., Dorjnamjaa, D., 1998. Relic permofrost structures in the Gobi of Mongolia: age and significance. Journal of Quaternary Science 13 (16), 539–548; Richards, B.W., Owen, L.A., Rhodes, E.J., 2000. Timing of Late Quaternary glaciations in the Himalayas of northern Pakistan. Journal of Quaternary Science 15, 283–297). In this paper, laboratory bleached samples from both the above studies are remeasured, using an experimental design to correct for OSL sensitivity changes, which has some similarities to the single aliquot regenerative dose (SAR) protocol of Murray and Wintle (Murray A.S., Wintle A.G., 2000. Luminescence dating of quartz using an improved single-aliquot regenerative-dose protocol. Radiation Measurements 32, 57–73). Clear evidence of thermal transfer OSL signals, generated during the preheating procedure, is presented. Further measurements, using the full SAR protocol, demonstrate that the source of this charge is related to natural dosing. For one sample, the apparent effect is subtracted effectively by the SAR protocol. Another sample studied in detail shows a striking relationship between the thermally transferred OSL signal and the total TL observed during the ramping of the preceding preheat treatment.     

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.     

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.     

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.     

On the dependence of equivalent dose on temperature of OSL measurements for sediment quartz grains and its implication in dating practice

The dependence of the equivalent dose (D_e) on the temperature used at stimulation when the standard OSL dating protocol (SAR) is applied has been investigated for sediment quartz samples. A considerable change in this value appears in the temperature region from 80 to 140 °C that is known for high complexity in OSL processes in quartz. Our observations suggest that the variation in the obtained results at least partly is caused by the laboratory procedure used when the natural OSL signal is measured. Directions for further investigations concerning this undesirable effect are indicated.     

Anomalous fading of the IRSL signal of polymineral grains in Chinese loess

Laboratory storage and preheating experiments were carried out to study anomalous fading of infrared stimulated luminescence (IRSL) signals derived from polymineral grains extracted from Chinese loess. Results of laboratory storage at 150 ^°C and higher temperature preheating experiments showed that such thermal treatments could lessen the effect of fading and indicated the presence of both thermal and non-thermal fading. In addition, the behavior of natural fading over the past 9–170 ka was investigated. By comparing with independent ages (obtained from fine-grain quartz using the optically stimulated luminescence (OSL) signal for the past 130 ka and the thermally transferred OSL (TT-OSL) signal in the age range of 130–170 ka) for the same samples, equivalent doses obtained from the IRSL signals were found to be underestimated by different amounts since the penultimate glacial; there was a linear dependence when the age underestimation was plotted against geological time.     

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.     

Optically stimulated luminescence production in the single-aliquot regenerative dose protocol

When using a single-aliquot regenerative dose (SAR) protocol for luminescence dating of sedimentary quartz grains, the fundamental assumption is that the sensitivity of the optically stimulated luminescence (OSL) produced by the regenerative doses can be monitored by their following test dose OSL response. Using well-bleached coarse quartz grains, OSL production in a SAR protocol was studied in detail when dose response curves were constructed using both single and multiple aliquot regenerative dose procedures. During application of the SAR protocol, two preheats are applied, each ahead of an OSL measurement that is produced by the regenerative dose and test dose, respectively. It is shown that sensitivity changes caused by heating were well corrected for using the OSL response to the test dose. However, these preheats are shown to result in thermally stimulated OSL signals that contribute both to the OSL response from the regenerative doses used to construct the dose response curve and to the OSL response from the test dose used to monitor OSL sensitivity changes as the quartz grains are repeatedly measured. A simple test is proposed to identify the contribution of the latter signal.     

TL/OSL properties of crystalline inclusions from heavy,barytes loaded,concrete

In the present work, we report the luminescence data obtained from heavy, barytes loaded, concrete containing many crystalline inclusions, extracted from a shielding block located at CERN. The use of both Thermoluminescence (TL) and Optically Stimulated Luminescence (OSL) signals, resulting from a specific trap at about 200 °C, is investigated for retrospective dosimetry purposes. By applying thermal cleaning experiments the TL signal of interest was isolated. Basic TL and OSL properties as thermal and optical stability, repeatability and mainly the linearity of the TL and OSL signals as a function of beta dose were investigated. The implications of all these luminescence properties to retrospective dosimetry are also briefly discussed.     

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.     

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

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

Luminescence dating of quartz using an improved single-aliquot regenerative-dose protocol

Single aliquot protocols are now widely used as a means of measuring the equivalent dose (D_e) in quartz and feldspar optical stimulated luminescence (OSL) dating of both heated and sedimentary materials. The most recent of these is the single-aliquot regenerative-dose (SAR) protocol, first suggested by Murray and Roberts (Radiation Measurements 29, 503–515, 1998). In this approach, each natural or regenerated dose OSL measurement is corrected for changes in sensitivity using the OSL response to a subsequent test dose (10–20% of D_e). If the sensitivity correction is adequate, then the corrected OSL response should be independent of prior dose and thermal/optical treatment, i.e. there should be no change in the sensitivity-corrected dose–response curve on remeasurement. Here we examine the interpretation of the sensitivity corrected growth curve as a function of dose, and the effect of changing measurement conditions (e.g. preheat temperature, size of test dose, stimulation temperature) on the estimation of D_e. The dependence of the dose response on prior treatment is tested explicitly, and the significance of thermal transfer discussed. It is concluded that a robust SAR protocol is now available for quartz, and that it is applicable to a wide range of heated and unheated materials.     

Improving the accuracy and precision of equivalent doses determined using the optically stimulated luminescence signal from single grains of quartz

Optically stimulated luminescence (OSL) measurements of quartz are widely used to measure equivalent dose (D_e). At radiation doses above ～100 Gy, saturation of traps results in a decrease in the rate of growth of the OSL signal, and this makes calculation of D_e increasingly difficult. A series of dose recovery experiments was undertaken using single grains of quartz from Kalambo Falls, Zambia to explore saturation of single grains. When the OSL signal from many grains is averaged, the characteristic dose (D₀) is 47 Gy, typical of published values for quartz. However, D₀ for individual grains varies from ～10 to 100 Gy. Doses up to two times the average D₀ could be accurately recovered, but above this dose the D_e became increasingly underestimated. Overdispersion for this type of experiment should be zero, but was observed in all data sets; furthermore the value of overdispersion increased with D_e. An additional acceptance criterion, the Fast Ratio, is suggested for single grain OSL analysis. This criterion assesses the relative contribution of the fast component of the OSL signal. Including this as an additional acceptance criterion leads to an improved precision, with overdispersion reduced to zero, and improved accuracy in dose recovery at high doses.