Red thermoluminescence (RTL) sensitivity change in quartz

This study investigated changes in the thermoluminescence sensitivity of volcanic and plutonic quartz following irradiation and annealing treatments with the aim of improving the accuracy of red thermoluminescence (RTL) dating. The response to X-ray irradiation (49 Gy) and RTL readout to 450 °C at a rate of 1 °C s^?1 was repeated 12 times and the sensitivity change induced by doses ranging from 49 to 293 Gy was examined. The results of these two experiments revealed that the final enhanced ratio of the sensitivity of plutonic quartz is 2.1–2.8 and 2.2–2.3 for two types of analyzed samples, much greater than that of volcanic quartz. To examine the thermal stability of quartz, several annealing treatments were performed from 300 to 900 °C for 100 min. An annealing treatment of 500 °C for 100 min resulted in a strong enhancement of RTL emission intensity for plutonic quartz, approaching the level for volcanic quartz. Finally, the single aliquot regeneration (SAR) method was applied to evaluate the absorbed dose, D_e, for aliquots irradiated with a known-dose ranging from 195 to 1952 Gy. All SAR D_e values obtained with volcanic quartz were in good agreement with the known dose values; whereas for plutonic quartz large uncertainties in D_e were obtained due to a marked sensitivity change. The magnitude of the RTL sensitivity change of quartz depends on dose and annealing treatment, and is clearly dependent on a classification of quartz based on thermal history.     

Yellow stimulated luminescence from potassium feldspar: Observations on its suitability for dating

Yellow stimulated luminescence (Y-OSL) is the light detected from potassium-rich feldspars at 410 nm under stimulation by a yellow light source emitting 590 nm. The investigation of this study aimed at understanding basic luminescence physics of Y-OSL in order to assess the suitability of the technique for dating. The Y-OSL signal properties tested were signal intensity, thermal assistance, thermal stability, sensitivity to daylight and the suitability of a single aliquot regenerative (SAR) protocol to be employed for equivalent dose (D_e) estimation. D_e measurements were conducted on samples of Holocene, last glacial and Tertiary age. The tests were undertaken on sedimentary feldspar separates extracted from aeolian, fluvial and coastal deposits.Results from experiments show that the signal intensity increases by measuring Y-OSL at elevated temperature suggesting thermal assistance characteristics similar to infrared stimulated luminescence (IRSL). The yellow stimulated signal remains unaffected by preheat temperatures up to ～200 °C suggesting higher thermal stability than the IRSL signal. The Y-OSL signal is less light sensitive than the IRSL signal and D_e residuals obtained from modern samples are up to 7 Gy indicating suitability of the technique for ‘older’ and well-bleached sediments. The dose recovery tests successfully recovered the given dose if the specific light sensitivity of Y-OSL is taken into account. For every sample Y-OSL D_e values obtained by a single aliquot regenerative dose protocol (SAR) are higher than those obtained by an IRSL SAR approach. From these results we infer high thermal stability and a minimal anomalous fading of the Y-OSL signal. We conclude that Y-OSL has a high potential to date Quaternary sediments that were sufficiently bleached in nature.     

Improving the TT-OSL SAR protocol through source trap characterisation

Thermally-transferred optically stimulated luminescence (TT-OSL) extends the age range of OSL dating using quartz. A set of experiments have been undertaken to determine the kinetic parameters of the TT-OSL source traps, and this information has been used to propose an improved TT-OSL single aliquot regenerative (SAR) dose protocol. By combining together OSL and thermoluminescence (TL) measurements on fine-grained quartz, a correspondence between TL peaks and the TT-OSL signal is found. The thermal stability of the main TT-OSL trap was estimated by applying Hoogenstraaten’s method and allowing for thermal quenching; this predicts a lifetime of 4.5 Ma at 10 °C. A set of experiments were undertaken to refine the treatment needed at the end of each SAR cycle to erase the previously acquired TT-OSL signal. An improved TT-OSL SAR protocol using this treatment is proposed, and it is tested on quartz from a young Holocene sample. These tests yielded excellent recycling ratios and excellent dose recovery.     

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.     

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.     

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.     

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.     

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.     

Using Zn as target to fabricate ZnO coating by thermal oxidation in air on quartz substrate

In this work, ZnO coatings were fabricated by the RF-sputtering method on quartz substrates in an inert gas ambient of Ar followed by a thermal oxidation process in air at different temperatures. The effect of thermal oxidation temperatures on the structures and photoluminescence (PL) properties of the coatings were studied. The structural characteristics of the samples were analyzed by X-ray diffraction (XRD) and atomic force microscope (AFM). The PL spectra were obtained by using a Xe laser as a light source with an excitation wavelength of 325 nm at room temperature. The force-curves were obtained by AFM. The results show that all the prepared ZnO coatings have a compact hexagonal wurtzite structure. With the increasing annealing temperature from 400 °C to 600 °C, the particle size, surface RMS roughness, photoluminescence intensity and adhesion force of the prepared ZnO coatings were increased as well.     

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.     

Luminescence lifetimes in quartz: dependence on annealing temperature prior to beta irradiation

It is well known that the thermal history of a quartz sample influences the optically stimulated luminescence sensitivity of the quartz. It is found that the optically stimulated luminescence lifetime, determined from time resolved spectra obtained with pulsed stimulation, also depends on past thermal treatment. For samples at 20°C during stimulation, the lifetime depends on beta dose and on duration of preheating at 220°C prior to stimulation for quartz annealed at 600°C and above, but is independent of these factors for quartz annealed at 500°C and below. For stimulation at higher temperatures, the lifetime becomes shorter if the sample is held at temperatures above 125°C during stimulation, in a manner consistent with thermal quenching. A single exponential decay is all that is required to fit the time resolved spectra for un-annealed quartz regardless of the temperature during stimulation (20–175°C), or to fit the time resolved spectra from all samples held at 20°C during stimulation, regardless of annealing temperature (20–1000°C). An additional shorter lifetime is found for some combinations of annealing temperature and temperature during stimulation. The results are discussed in terms of a model previously used to explain thermal sensitisation. The luminescence lifetime data are best explained by the presence of two principal luminescence centres, their relative importance depending on the annealing temperature, with a third centre involved for limited combinations of annealing temperature and temperature during stimulation.     

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.     

Identifying well-bleached quartz using the different bleaching rates of quartz and feldspar luminescence signals

When dating older sedimentary deposits using quartz, there are no unambiguous methods for identifying the presence of incomplete bleaching. Current statistical analysis of dose distributions depends entirely on the assumption that incomplete bleaching and mixing are the main causes of any excess dispersion in the distribution; the only existing way to test this assumption is using independent age control. Here we suggest a new approach to this question, based on the differential bleaching rates of quartz and feldspar luminescence signals. We first present data that confirm the differences in relative bleaching rates of quartz optically stimulated luminescence (OSL) and feldspar luminescence stimulated at 50 °C by infrared light (IR₅₀) and feldspar luminescence stimulated at 290 °C by infrared light after a stimulation at 50 °C (pIRIR₂₉₀), and use recently deposited samples to determine the likely significance of the difficult-to-bleach residual feldspar signals in non-aeolian samples. For a set of mainly Late Pleistocene non-aeolian sediments, large aliquot quartz doses are then used to predict feldspar doses (based on a knowledge of the sample dose rates). The differences between observed and predicted feldspar doses as a function of the quartz dose, combined with a conservative assumption concerning the relative feldspar and quartz residual signals after natural bleaching prior to deposition, are used to identify those samples for which the quartz is very likely to be well bleached (20 out of 24). Two of these apparently well-bleached samples are then examined using single-grain quartz dose distributions; one of these is consistent with the well-bleached hypothesis, and one indicates poor bleaching or a multi-component mixture. However, independent age control makes it clear that the large aliquot data are more likely to be correct. We conclude that a comparison of quartz and feldspar doses provides a useful independent method for identifying well-bleached quartz samples, and that it is unwise to apply statistical models to dose distributions without clear evidence for the physical origins of the distributions.     

On the intrinsic accuracy and precision of the standardised growth curve (SGC) and global-SGC (gSGC) methods for equivalent dose determination: A simulation study

In optically stimulated luminescence (OSL) dating, the single aliquot regenerative-dose (SAR) method has been used extensively for determining equivalent doses (D_e) in quartz. A variation of the SAR method is the “standardised growth curve” (SGC) method, which has been used as an efficient procedure to save measurement time during dating studies. During the application of the SGC method one establishes the SGC and calculation of the D_e of an aliquot requires only measurement of the standardised natural dose signal. Recently, a “global standardised growth curve” (gSGC) method was developed as an improved version of the SGC procedure. During the application of the gSGC method, the growth curves are re-normalised using sensitivity-corrected signal corresponding to one of the regenerative doses. Subsequently the D_e of an aliquot is estimated using the sensitivity-corrected natural dose signal and an additional sensitivity-corrected regenerative dose signal as well as the established gSGC. In the present study, simulations are performed to assess the intrinsic accuracy and precision of the SGC and gSGC D_e estimates. The results of our simulations validate that the gSGC method is intrinsically more precise than the SGC method and is also more accurate for doses greater than 210 Gy. Several factors which affect the reliability of the two methods are investigated.     

Using the OSL single-aliquot regenerative-dose protocol with quartz extracted from building materials in retrospective dosimetry

We report on the application of the single-aliquot regenerative-dose (SAR) protocol to the optically stimulated luminescence signal from quartz extracted from fired bricks and unfired mortar in retrospective dosimetry. The samples came from a radioactive materials storage facility, with ambient dose rates of about 0.1 mGy/h. A detailed dose-depth profile was analysed from one brick, and compared with dose records from area TL dosemeters. Small-aliquot dose-distributions were analysed from the mortar samples; one associated with the exposed brick, and one from a remote site exposed only to background radiation. We conclude that unfired materials have considerable potential in retrospective dosimetry.     

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

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

Natural variations in the properties of TL and IRSL emissions from metamorphic and volcanic K-feldspars from East Africa: Assessing their reliability for dating

The elevated temperature infrared stimulated luminescence (IRSL) and post-IR IRSL signals of potassium (K)-feldspars have recently garnered attention for their minimal rates of anomalous fading. The post-IR IRSL signal has been used to obtain age estimates for geological deposits, mostly in Europe. Studies on the behaviour of the IRSL and post-IR IRSL signals of K-feldspars from a wider range of geographic regions and depositional contexts are needed, particularly for regions where the OSL signal from quartz is poorly behaved. Discrepancies in the literature regarding the behaviours of the IRSL and TL signals of K-feldspars also highlight the need to characterise the behaviours of samples from a wide variety of contexts. This paper begins to address this problem by characterising and comparing the IRSL signals of a metamorphic and a volcanic K-feldspar sample from two sites in East Africa, a region in which the OSL signal from quartz has generally proven problematic for dating. We demonstrate that the metamorphic and volcanic K-feldspars have substantially different TL glow curves that respond differently to IR stimulation. The sample of metamorphic K-feldspar from Tanzania (MR9) has a peak at 430 °C that is associated with the IRSL signal and an optically less-sensitive peak at 350 °C, while the sample of volcanic K-feldspar from Ethiopia (MB3) exhibits a single broad TL region centred at ～230 °C that responds differently to IR stimulation. Differences in the change of IRSL decay curve shape with stimulation temperature suggest that the processes of IRSL production many vary between the two samples. Using dose recovery tests, we demonstrate that the IRSL (50 °C), IRSL (225 °C) and post-IR IRSL (50 °C, 225 °C) signals of sample MR9 are suitable for dose and age estimation using the single-aliquot regenerative-dose procedure, while those of sample MB3 are less suitable. The post-IR IRSL signal of the latter sample performs poorly in tests of SAR suitability and the three signals exhibit extremely high fading rates over laboratory timescales (g_2days > 19%/decade).     

Standardised growth curves for optical dating of sediment using multiple-grain aliquots

The single aliquot regenerative dose (SAR) protocol offers the opportunity of exploring, relatively simply, the existence of a ‘universal’ growth curve for use in dating using optically stimulated luminescence (OSL). A test dose is used in the SAR procedure to monitor and correct for sensitivity change occurring either over the burial period, or as a result of thermal pretreatments during the measurement procedure. However, this test dose can also be used to correct for variations in signal intensity between individual aliquots, thus enabling the comparison of growth response with dose for many different aliquots and samples, even for measurements made using different instruments.In this paper, the growth characteristics of coarse-grained quartz and polymineral fine-grains are examined using data obtained as part of the SAR procedure. Following standardisation of these data for differences in the test dose response and the magnitude of the test dose used, distinct and reproducible patterns of growth are observed and mineral-specific standardised growth curves (SGCs) are defined for multiple-grain aliquots. An equivalent dose for a sample can then be determined based only on measurements of the natural luminescence signal intensity (L_n) and the response to an artificial irradiation dose (T_n). This equivalent dose, determined using the SGCs defined for quartz and polymineral fine-grains, is compared to that determined using a conventional SAR measurement procedure, for a large number of samples and aliquots. Using an SGC, accurate estimates of equivalent dose may be made based solely on measurements of L_n and T_n, thus potentially speeding up the measurement process. This has obvious benefits where it is necessary to examine a large number of aliquots.     

The effect of heat treatment on the thermoluminescence of naturally-occurring calcites and their use as a gamma-ray dosimeter

The feasibility of using naturally-occurring calcite for gamma-ray dosimetry was investigated. Anneal treatment above 350°C increased the sensitivity of all radiation-induced TL peaks except the glow peaks above 300°C. On the other hand, annealing in air, at a temperature of 700°C caused a collapse in the TL sensitivity. The increase in TL efficiency was found to depend on the annealing temperature and time. Heating at 600°C for 5 h and quenching in ambient air are the optimum conditions for TL sensitivity enhancement in the calcite materials investigated. These results are explained using the energy scheme of the pre-dose model of Zimmerman (1971) and in terms of the impurity rearrangements in the crystal lattice induced by heating. It was found that the values of the kinetic parameters E, s and b for TL glow peaks remained unchanged for annealed samples. The TL dose–response curves for stable dosimetric peaks of annealed and unannealed calcite samples could be fitted to the same linear mathematical function. This implies that the annealing process probably does not change the nature of the trapping centers except the low temperature TL peaks at 125 and 160°C of flowstone. The TL dosimetric parameters of calcite samples annealed, including glow curves, fading characteristics, dose–responses, dose-rate responses and energy responses, have also been studied in detail. The response to gamma-rays of annealed calcite samples was found to be linear from 0.05 to 10⁴ Gy. The lower limit of observable doses for each calcite sample was about 0.05 Gy. This offers the possibility of applying the investigated materials for gamma-ray dosimetry within this useful range. These dosimeters can be used in various applications, such as, in industries related to chemical technology (polymerization), food processing and in determining the dose received by the patient during medical examination and treatment.