Luminescence dating: laboratory procedures and protocols

In the last 30 years, from 1967 to 1997, the use of luminescence signals from naturally occurring minerals has gone though a major metamorphosis, from thermoluminescence (TL) dating of pottery to optically stimulated luminescence (OSL) dating of sediments. Laboratory procedures for dating sediments have been adapted from those for pottery and new procedures have been developed as the need arises.

The majority of sediment dating applications are carried out on quartz and potassium-rich feldspars and the general characteristics of the TL and OSL signals from these minerals are reviewed. For sediments some new problems were encountered, with some grains perhaps not being completely bleached at deposition. For OSL signals there is no simple procedure for the selection of a thermally stable signal, as there had been in the case of pottery.

Many different laboratory protocols have been developed as our understanding of the fundamental behaviour of luminescence signals from quartz and feldspar has improved. These protocols are explained and discussed, giving the advantages and disadvantages of each procedure as applied to different types of sediment.

This review is presented as a guide to the selection of the most appropriate procedure for a particular dating application.     

Crushing effects on TL and OSL on quartz: relevance to fault dating

The effect of crushing on the TL and OSL signals in quartz was investigated to examine the feasibility of using OSL and TL for dating of faulted rocks. 275°C TL signals were not reduced by crushing by hand (mortar and pestle), in a pellet die press, or using an automatic mortar and pestle, but the sensitivity of the 100°C TL signal to a test dose decreased in crushed samples. Green light-stimulated OSL signal intensities were not decreased after crushing, but showed strongly increased inter-aliquot variability after crushing. We concluded that OSL and TL in quartz might be useful to characterize the crushing history of quartz in fault rocks, but their usefulness in dating fault events was not evident because we did not find evidence of signal zeroing under the conditions used in this study.     

Study of sensitivity change of OSL signals from quartz and feldspars as a function of preheat temperature

Optically stimulated luminescence (OSL) signals from feldspar and quartz samples were studied using infrared (860 nm) and green light (420–575 nm) stimulation. A serious problem connected with the regeneration technique used for dating is associated with a change of OSL sensitivity to radiation in the course of the measurement process. A typical effect seen is a large increase of the apparent strength of our beta source when calibrated against a gamma source. If the regeneration procedure is used, it is shown that the sensitivity increases up to 50% during the measurement process and as a result, the equivalent dose (ED) would be underestimated. A study of sensitivity changes in feldspars and quartz was carried out with emphasis on the effect of preheat and annealing on the OSL signal. Measurement results obtained are presented, and possible elimination of errors in dating caused by sensitivity changes is discussed.     

The timing of OSL sensitivity changes in a natural quartz

The timing of 110°C thermoluminescence (TL) and optically stimulated luminescence (OSL) sensitivity changes is explored using a natural (aeolian) quartz sample from Australia that was previously found to exhibit marked dose-dependent sensitivity change. The changes occur asynchronously; the 110°C TL sensitivity changes after dosing plus pre-heating, whereas the OSL sensitivity changes (proportionately with dose) after optical bleaching. Although the magnitude and saturation characteristics of the sensitivity changes are found to be similar, their non-synchronicity negates a direct link between the phenomena. Implications of these results for dating procedures are discussed. In particular, the results indicate that a single aliquot additive dose procedure similar to that developed for coarse-grained potassium feldspar should be possible for some quartz samples.     

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.     

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.     

Behavioural studies of stimulated luminescence from feldspars

Since the work of Mejdahl in the mid-1980s feldspars have been used widely for palaeodosimetry. They have proved particularly popular because of the technical ease with which an optically stimulated luminescence signal can be obtained, and the potential for their use in dating over a wider time range than quartz. However, while the use of infrared stimulated lminescence has been a great success, the realisation of the potential for dating over a wide time range has been hampered by a series of behavioural problems, in particular concerned with the stability of the luminescence signal. This paper surveys the current state of knowledge of a range of aspects of the stimulated luminescence behaviour of feldspar. Particular attention is paid to the thermal and optical properties of the thermoluminescence (TL) and optically stimulated luminescence (OSL) signals from feldspars since these are of greatest relevance to their use as palaeodosimeters. Results obtained from well-characterised museum specimens demonstrate the variety of responses that are seen from different types of feldspar, particularly in their TL behaviour. Less variation is seen in their OSL response. In contrast, the response of potassium-rich feldspars separated from Quaternary sediments tends to be very consistent when many grains are analysed simultaneously, suggesting that averaging of the signal simplifies the behaviour of the system.     

A survey of the signal stability and radiation dose response of sulfates in the context of adapting optical dating for Mars

The Martian landscape is currently dominated by eolian processes, and eolian dunes are a direct geomorphic expression of the dynamic interaction between the atmosphere and the lithosphere of planets. The timing, frequency, and spatial extent of dune mobility directly reflects changing climatic conditions, therefore, sedimentary depositional ages are important for understanding the paleoclimatic and geomorphologic history of features and processes present on the surface of the Earth or Mars. Optical dating is an established terrestrial dosimetric dating technique that is being developed for this task on Mars. Gypsum and anhydrite are two of the most stable and abundant sulfate species found on the Earth, and they have been discovered in Martian sediments along with various magnesium sulfates and jarosite. In this study, the optical dating properties of various Ca-, Mg-, and Fe-bearing sulfates were documented to help evaluate the influence they may have on in-situ optical dating in eolian environments on Mars. Single-aliquot regenerative-dose (SAR) experimental procedures have been adapted to characterize the radiation dose response and signal stability of the Martian sulfate analogs. Jarosite was dosimetrically inert in our experiments. The radiation dose response of the Ca- and Mg-sulfates was monotonically increasing in all cases with characteristic doses ranging from ∼100 to ∼1000 Gy. Short-term signal fading also varied considerably in the Ca- and Mg-sulfates ranging from ∼0% to ∼40% per decade for these materials. These results suggest that the OSL properties of Ca- and Mg-sulfates will need to be considered when developing protocols for in-situ optical dating on Mars, but more enticingly, our results foreshadow the potential for gypsum to be developed as a geochronometer for Mars or the Earth.     

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.     

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.     

Empirical insights into multi-grain averaging effects from ‘pseudo’ single-grain OSL measurements

In this study we assess the signatures of multi-grain averaging effects for a series of sedimentary samples taken from the archaeological site of Hotel California, Atapuerca, Spain. We focus on the special case of equivalent dose (D_e) measurements made on single-grain discs that contain more than one quartz grain in each of the individual grain-hole positions with the aims of (i) providing insight into the nature and extent of averaging effects in very small multi-grain aliquots of sedimentary quartz, and (ii) assessing the suitability of ‘pseudo’ single-grain D_e measurements for this particular dating application. Pseudo single-grain OSL measurements made on standard discs loaded with 90–100 μm grains (equivalent to ～30 grains per hole) yield significantly different D_e distribution characteristics and finite mixture model (FMM) burial dose estimates compared with single-grain OSL measurements. Grains with aberrant luminescence behaviours, which are routinely rejected during single-grain analysis, exert strong averaging effects on the pseudo single-grain and multi-grain aliquot D_e distributions. Grain-hole averaging effects arising from pseudo single-grain measurements also give rise to ‘phantom’ dose components and are apt to provide bias assessments of quartz signal characteristics and grain type classifications. Though this is a site-specific study, it serves as a cautionary note for interpretations of other pseudo single-grain OSL and D_e datasets – particularly those obtained from measurements of discs containing several tens of grains per hole and those derived from complex depositional environments. The use of custom single-grain discs drilled with smaller sized grain holes is recommended as a means of limiting grain-hole averaging effects when dealing with very fine (<180 μm) 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.     

Kinetics of red, blue and UV thermoluminescence and optically-stimulated luminescence from quartz

The duration over which charge is retained at trapping sites is of fundamental importance for trapped electron dating. Here, we report measurements of the kinetic parameters of the prominent thermoluminescence (TL) glow peaks of quartz, and of the optically-stimulated luminescence (OSL) signal from quartz utilised for optical dating. The similarity in trapping lifetimes of the 325°C TL peak and the dominant component of the OSL signal are taken as further support for the hypothesis of their common origin in the same trapped electron population.     

The effects of low ambient temperatures on optically stimulated luminescence (OSL) processes: Relevance to OSL dating of martian sediments

Advances in luminescence dosimetry have made geochronological dating of materials from extreme environments possible through the use of optically stimulated luminescence (OSL) single-aliquot techniques. However, these environments present challenges not always encountered in routine OSL dating, such as sediments that have been stored at low, and possibly highly variable, ambient temperatures. In recent years OSL has been proposed as a method for dating recent depositional events on surfaces of other planets, specifically, Mars. As a result it has become necessary to examine the constraints that may be imposed on the OSL method by the extreme environments of extraterrestrial planetary bodies. In this paper we report on investigations of the possible effects a low storage and/or a low OSL measurement temperature could have on the OSL process and the subsequent results. Pertinent OSL properties include the stability of electron traps, the overall luminescence efficiency, and possible thermal assistance processes. The particular focus of the work is on the potential application of the OSL technique for dating surface sediments on Mars. We report the results of OSL experiments on martian simulant materials, and of generalized computer simulations of potential OSL behavior. It is concluded that the stimulation and irradiation/calibration temperatures need to be maintained fixed throughout the experiment – i.e. the dose estimation process – and that the temperature during OSL stimulation needs to be appreciably higher than the highest temperature experienced during natural irradiation. The consequences of these findings for establishing an OSL protocol and instrument package for dating martian regolith material are discussed.     

Fluvio-mechanical resetting of the Al and Ti centres in quartz

ESR dating of fluvial terraces is usually based on the assumption of sunlight resetting of the Al centres in quartz. Very long bleaching times (months of sunlight exposure) are required to reset this centre to a stable, non-zero ESR intensity. Considering that highly light sensitive optically stimulated luminescence (OSL) analyses of fluvial samples often indicate partial bleaching, ESR dating should be extremely difficult. Two samples were analysed, a fluvial sediment from a Chinese river terrace and an Australian granite. Using a Höhnle sunlight simulator, the Ti centres of both samples were completely bleached within 1 to 65 h, while the Al centre required extreme bleaching times to reach stable residual intensities (∼1000 h). As an alternative to light resetting, tumbler experiments were carried out to simulate fluvial action. The samples were treated under OSL sample preparation conditions. After relatively short tumbling times, corresponding to a few km of fluvial transport, both Al- and Ti-centres were partially reset. In a granite sample, the tumbling reduced the intensity of the Al centre more effectively than light exposure.     

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.     

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.     

Use of the LM-OSL technique for the detection of partial bleaching in quartz

We present a study of the sensitivity to light (ease-of-bleaching) of the trapped charge in sedimentary quartz grains using an optically stimulated luminescence (OSL) technique in which the intensity of the stimulation light is linearly increased during the measurement period. The technique is known as linear modulation OSL (LM-OSL). In controlled laboratory conditions, this technique has been employed to study the ease-of-bleaching of the trapped charge in quartz by comparing the OSL curves of quartz aliquots which have been either: (1) fully bleached, followed by a laboratory dose of β-irradiation, or (2) partially bleached, followed by the laboratory β-dose. The ratio of the OSL signals due to the β-dose from the partly and fully bleached aliquots is illustrated to be a potential indicator of the degree of optical resetting of the OSL signal in dating material. The key parameter governing the ease-of-bleaching is the photoionization cross-section of the trap involved. The concept is also demonstrated in a model study from which very good agreement with the experimental observations has been found. Potential applications of the technique to dating are discussed.     

The interpretation of quartz optically stimulated luminescence equivalent dose versus time plots

Numerical modelling has shown that the form of the quartz OSL shine plateau (hereafter ‘D_e(t)-plot’) is influenced by the effects of phototransferred TL in the ∼110°C region. It is suggested also that the presence of multiple OSL components (as described by Bailey, Smith and Rhodes, 1997. Partial bleaching and the decay form characteristics of quartz OSL. Radiat. Meas., 27, 123–136; Bailey, 1998. The form of the optically stimulated luminescence signal of quartz: implications of dating. Unpublished PhD thesis, University of London) affects the form of the D_e(t)-plot. Laboratory measurements of a fully reset and artificially dosed sample yielded non-flat D_e(t)-plots, the deviation being greater for the larger of the two simulated palaeodoses, in accordance with theoretical predictions. It is suggested that the so-called ‘shine plateau’ test is of limited use in assessing the bleaching history of quartz sediments.     

Luminescence sensitivity changes in quartz as a result of annealing

Retrospective dosimetry using optically stimulated luminescence (OSL) on quartz extracted from (for example) bricks needs to account for strong OSL sensitivity changes that are known to occur depending on the previous thermal treatment of the sample. Non-heated quartz exhibits OSL orders of magnitude less per unit radiation than that for heated material. The reason these temperature-induced sensitivity changes occur in quartz is presently not well understood. This phenomenon is also seen in the related area of luminescence dating in which sedimentary quartz and quartz from heated archaeological samples show very different OSL sensitivities. In this paper we report on studies of the effects of high temperature annealing on the OSL and phototransferred TL (PTTL) signals from sedimentary and synthetic quartz. A dramatic enhancement of both OSL and PTTL sensitivity was found especially in the temperature range 500–800°C. Computer simulations of the possible effects are shown to produce data that agree in all essential details with the experimental observations. It is further demonstrated that the enhanced OSL sensitivity as a function of annealing temperature is not a pre-dose effect.