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.     

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).     

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.     

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.     

Luminescence property of volcanic quartz and the use of red isothermal TL for dating tephras

An optically stimulated luminescence (OSL) age obtained from a Japanese tephra using quartz phenocrysts severely underestimated the known age. The characteristics of the OSL signals were investigated in order to understand the cause of the underestimation; the main OSL component of volcanic quartz has a thermodynamic lifetime of about 1700 years at room temperature, and it also seems to fade anomalously (i.e. athermally). Measurement of conventional red thermoluminescence (RTL) using a Ga–As photomultiplier tube was difficult due to the presence of a strong thermal background, although RTL gave an age consistent with the independent age. Furthermore, red isothermal TL (RITL) at 380 °C allowed the RTL signal to be separated from to the thermal background, and RITL ages of three volcanic quartz samples show good agreement with independent ages.     

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.     

Investigating signal evolution: A comparison of red and UV/blue TL,and UV OSL emissions from the same quartz sample

Samples from plutonic geological settings emit strong and stable UV, blue and red luminescence. These samples provide a unique opportunity to investigate the evolution of luminescence emissions by comparing their origin, intensity, trapping and recombination characteristics. In addition, the D_e derived from certain techniques can be used to investigate D_e consistency. Thus, UV and red signals emitted by the same sample of grantic quartz have been compared according to the strength and shape of the emissions, response to annealing and dose, growth characteristics and the resulting D_e derived from single-aliquot regeneration (SAR – UV emissions) and the dual-aliquot protocol for red TL (DAP – red emissions). This comparison of UV and red D_e values can be used as an alternative measure of accuracy for depositional situations where independent age control is not available. Furthermore, this comparison has been extended to a single-grain level to determine if UV and red signals are emitted by the same quartz grain. The resulting comparisons demonstrate that both signals are strong, reproducible, are suitable for dating, and a comparison of D_e is a valid internal check of consistency. The single-grain analysis demonstrates that the grains contain UV and red recombination centres rather than the typical characteristics of just beta or alpha quartz. Thus it has been suggested that the emissions relate to post-origin modifications of the signal rather than its thermal origin. This type of comparative analysis provides clues as to the source and evolution of the signals, provides a greater understanding of the complexities of the luminescence signal and a possible solution for accuracy testing in challenging depositional contexts.     

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.     

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.     

Gamma ray induced sensitization of 110°C TL peak in quartz separated from sand

We have investigated the gamma ray induced sensitization of the 110°C TL peak in quartz, separated from sand, in the dose range 30–750 Gy. A pre-dose of 100 Gy followed by annealing at 500°C for 1 h yielded an optimum sensitization factor of 14.2 for a test gamma dose of 0.5 Gy; this factor decreases slowly up to the studied pre-gamma dose of 750 Gy. From ESR studies carried out in the temperature range 25–550°C, the formation of E′₁-centres and their subsequent decay (at temperatures >400°C) have been observed. The released charge carriers (electrons) may lead to elimination of competitors (as a result of their filling up). Thus, the radiation-induced sensitization of the 110°C TL peak could be due to elimination of the competing deep traps.     

Effect of annealing on natural calcitic crystals—A thermostimulated luminescence (TSL) study

The quality crystals (Calcitic limestone) were selected using the UV–visible methylene blue adsorption method. The thermostimulated luminescence (TSL) glow curve characteristics of six well crystallized limestone samples were analyzed. The glow curves of unannealed sample show only one peak in the range 320–330 °C. The sample irradiated with a gamma dose of 100 Gy shows two additional peaks in the range of 113–125 °C and 242–260 °C when recorded with linear heating rate of 10 °C/s. The annealed sample also shows the same trend as that of irradiated sample. Annealing treatment above 250 °C increases the sensitivity of all TSL peaks except 320 °C. On the other hand, annealing at 750 °C caused a collapse in the TSL sensitivity. The enhancement in TSL sensitivity was found to depend on the annealing temperature and time. Annealing treatment at 650 °C for 4 h followed by quenching in air is the optimum condition for TSL sensitization. The response to gamma irradiation is linear in the range from 0.5 Gy to 10⁴ Gy. The emission spectra of all the samples show an emission at around 610 nm but with different intensities for each TSL peak. With reference to earlier work, it may be assumed that the recombination site always involves Mn²⁺ ions. The observation made through infra-red (IR) and X-ray diffraction (XRD) studies with thermal treatment shows the structural changes of calcite from D_3h to C_s symmetry at 750 °C. The Thermogravimetric-Differential Thermal Analysis (TG-DTA) analysis shows the calcite gets disordered at 760 °C. Hence, the collapse in the TSL sensitivity at 750 °C is due to structural change or structural disorderedness.     

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.     

Investigations of the post-IR IRSL protocol applied to single K-feldspar grains from fluvial sediment samples

The post-IR IRSL protocol with single K-feldspar grains was applied to three samples taken from a fluvial sedimentary sequence at the archaeological site of the Dali Man, Shaanxi Province, China. K-feldspar coarse grains were extracted for measurement. Approximately 30–40% of the grains were sufficiently bright to measure, and after application of rejection criteria based on signal strength, recuperation, recycling ratio and saturation dose, ～10–15% of the grains were used for D_e calculation. The relationship of signal decay rate and form of D_e(t) with the recovery dose were investigated. The dose recovery ratios of the samples after initial bleaching with the four different light sources were within uncertainties of unity. No anomalous fading was observed. The over-dispersion of the recovered dose and D_e values were similar, suggesting neither incomplete resetting of the post-IR IRSL signals nor spatially heterogeneous dose rates significantly affected the natural dose estimates. The values of D_e obtained with the single K-feldspar grain post-IR IRSL protocol were in the range ～400–490 Gy. Combining all of the measured single-grain signals for each of the individual samples (into a ‘synthetic single aliquot’) increased the D_e estimates to the range ～700–900 Gy, suggesting that the grains screened-out by the rejection criteria may have the potential to cause palaeodose over-estimation, although this finding requires a more extensive investigation. Thermally transferred signals were found in the single K-feldspar grains post-IR IRSL protocol, and the proportion of thermally transferred signal to test-dose OSL signal (stimulation at 290 °C) from the natural dose was higher than from regenerative doses, and the proportion was grain- and dose-dependent. As such, TT-post-IR IRSL signals at 290 °C have the potential to cause dose underestimation, although this may be reduced by using larger test-dose irradiations. Our study demonstrates considerable potential in the post-IR IRSL method in providing chronological control in studies relevant to human evolution in the later-Pleistocene.     

Thermoluminescence characterization of the Cu(Tb,Tm)-12CaO-7AL2O3 compounds obtained by combustion synthesis

The thermoluminescence (TL) properties of dode-calcium hepta-aluminate (Ca₁₂Al₁₄O₃₃) enabled by 12CaO-7Al₂O₃ doped with rare earth and transitions metals ions have been studied and their suitability for radiation dosimetry applications is discussed. It was observed that this calcium aluminate phase doped with Tm-Cu at concentration of 0.1 mol% is a good candidate for dosimetric applications since it presents well-defined single peak observed at 240 °C and 320 °C and a linear response to gamma radiation dose from 5 × 10⁻³ Gy up to 100 Gy.     

Luminescence sensitivity changes of quartz by bleaching,annealing and UV exposure

The sensitivities of quartz luminescence signals to dose were studied after ionizing irradiation, ultraviolet (UV) exposure and different annealing conditions. The relationship between the 110 v °C thermoluminescence (TL) and optically stimulated luminescence (OSL) were studied on the same aliquot by looking at the ratio of both signals created by a test dose. It is suggested that the sensitivity changes of both signals are closely related, but not identical. Significant differences are observed when annealing to temperatures higher than 500 v °C. A modified model was proposed to interpret the observations. The similarity is interpreted as the same R hole centers are shared by both signals, whereas 110 v °C TL only uses additional R hole centers. Dramatic changes in luminescence sensitivity for quartz relate to the phase changes.     

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.     

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.     

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.     

Extending the time range of luminescence dating using red TL (RTL) from volcanic quartz

The potential of red thermoluminescence (RTL) emission from quartz, as a dosimeter for baked sediments and volcanic deposits, has received some attention over the past decade. While there have been some important observations relating to signal stability, saturation characteristics and emission wavebands, there has not been a systematic analysis of RTL properties of older (i.e., >1 Ma), quartz-bearing known age volcanic deposits. We have undertaken such an analysis using independently-dated silicic volcanic deposits from New Zealand, ranging in age from 300 ka through to 1.6 Ma. We observed a complex RTL emission in most volcanic quartzes, which consists of a number of discrete high temperature (i.e, >220°C) TL peaks. Isothermal analysis indicates a stable dating trap (E=2.03 eV; S=4.20×10¹⁵) which is stable at ambient (c. 20°C) temperatures for >10⁹ a. We confirm the slow onset of saturation with dose, and the limited extent of sensitivity changes due to dosing and TL readout. As such, there is much potential for exploiting the dosimeter in dating studies and we present the results from a modified single aliquot regenerative (SAR) procedures which indicate that there is a good agreement between RTL dating and other methods over time scales 10⁵–10⁶ a. This paper presents a summary of the most important related results of our findings and outlines the configuration of photomultiplier and filter combinations which maximizes RTL detection for temperatures up to 500°C.     

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).