Review and assessment of the potential of post-IR IRSL dating methods to circumvent the problem of anomalous fading in feldspar luminescence

Quartz has been the main mineral used for optically stimulated luminescence (OSL) dating of sediments over the last decade. The quartz OSL signal, however, has been shown to saturate at relatively low doses of ～200–400 Gy, making it difficult to be used for dating beyond about 200 thou-sand years (ka), unless the environmental dose rate is low. The infrared stimulated luminescence (IRSL) from feldspars has been shown to continue to grow to higher dose levels than quartz OSL. The application of IRSL dating of feldspars, however, has long been hampered by the anomalous fading effect. Recent progress in understanding anomalous fading of the infrared stimulated luminescence (IRSL) signals in potassium-feldspar has led to the development of post-IR IRSL (pIRIR) protocols and also a multiple elevated temperature (MET) stimulation (MET-pIRIR) protocol. These procedures have raised the prospect of isolating a non-fading IRSL component for dating Quaternary deposits containing feldspars. In this study, we review the recent progress made on (1) overcoming anomalous fading of feldspar, and (2) the development of pIRIR dating techniques for feldspar. The potential and problems associated with these methods are discussed.     

On the applicability of post-IR IRSL dating to Japanese loess

Recent work on infrared stimulated luminescence (IRSL) dating has focussed on finding and testing signals which show less or negligible fading. IRSL signals measured at elevated temperature following IR stimulation at 50°C (post-IR IRSL) have been shown to be much more stable than the low temperature IRSL signal and seem to have considerable potential for dating. For Early Pleistocene samples of both European and Chinese loess natural post-IR IRSL signals lying in the saturation region of the laboratory dose response curve have been observed; this suggests that there is no significant fading in nature. As a contribution to the further testing of post-IR IRSL dating, we have used 18 samples from two Japanese loess profiles for which quartz OSL and tephra ages up to 600 ka provide age control. After a preheat of 320°C (60 s), the polymineral fine grains (4–11 μm) were bleached with IR at 50°C (200 s) and the IRSL was subsequently measured at 290°C for 200 s. In general, the fading uncorrected post-IR IRSL ages agree with both the quartz OSL and the tephra ages. We conclude that the post-IR IRSL signal from these samples does not fade significantly and allows precise and accurate age determinations on these sediments.     

IRSL and post-IR IRSL residual doses recorded in modern dust samples from the Chinese Loess Plateau

Using a set of modern/young (0 to about 200 years old) dust samples collected from the Chinese Loess Plateau the bleachability of IRSL measured at 50°C (IR₅₀) and post-IR₅₀ elevated temperature IRSL (measured at 225°C and at 290°C) is investigated by measuring the apparent (residual) doses recorded by these signals. Doses recorded by quartz OSL are used as a reference. Allowing for differences in dose rates it seems that both IRSL and post-IR IRSL signals yield residual doses that are significantly larger than the doses measured in quartz. These residual doses can be largely explained by thermal transfer caused by preheating. Nevertheless, we advise against the use of a low temperature preheat (<200°C) with IR₅₀ to date loess samples because, as has been reported before, the signal appears to be thermally unstable. In general, we conclude that it may not be advisable to apply post-IR IRSL dating to Chinese loess samples where residuals of up to ∼20 Gy are a significant fraction of the total dose. However, these residuals quickly become unimportant when dating older samples, and this is the age range in which post-IR IRSL dating is likely to be most useful.     

Luminescence dating of volcanogenic outburst flood sediments from Aso volcano and tephric loess deposits, southwest Japan

Luminescence dating has been applied to volcanogenic outburst flood sediments (Takuma gravel bed) from Aso volcano, Japan, and tephric loess deposits overlying the gravel bed. The poly-mineral fine grains (4–11 μm) from loess deposits were measured with pulsed optically stimulated luminescence (pulsed OSL) and post-IR infrared stimulated luminescence (pIRIR) methods, whereas the Takuma gravel bed containing no quartz, was measured with IRSL and pIRIR methods using sand sized (150–200 μm) plagioclase. The loess deposits date back at least to ～50 ka by consistent IRSL, pIRIR and pulsed OSL ages from the lowermost part of the loess deposits from one section. The ages obtained from the bottom part of the other loess section are not consistent each other. However, we consider that the pIRIR age (72±6 ka) which showed negligible anomalous fading is most reliable, and regard as a preliminary minimum age of the Takuma gravel bed. The equivalent doses (D_e) for the plagioclase from the Takuma gravel bed have a narrow distribution and the weighted mean of the three samples yield an age of 89±3 ka. This age is in agreement with the last caldera-forming eruption of Aso volcano (～87 ka) and it is likely that the pIRIR signal has not been bleached before the deposition. IRSL dating without applying pIRIR using small aliquots was also conducted, however, the IRSL signal shows no clear evidence of an additional bleaching during the event of outburst flood from the caldera lake.     

Stability of IRSL signals from sedimentary K-feldspar samples

Recent work has identified IR stimulated luminescence signals at elevated temperature from both potassium- and sodium-rich feldspars that have much lower anomalous fading rates than the conventional signal measured using IR stimulation at 50°C. This paper examines the stability of these signals for potassium-rich sedimentary feldspars. We show that the natural post-IR IRSL (pIRIR) signal from a 3.6 Ma old sample is in apparent saturation on a laboratory generated dose response curve, i.e. it does not show detectable fading in nature although a low fading rate is observed on laboratory time scales. We show that the pIRIR signal has a greater thermal stability than the IRSL signal and that the trend in increasing thermal stability is mirrored by a decreasing fading rate. We also investigate the effect of preheat temperature and IR stimulation power on the decay shape and conclude that the data can be explained in terms of either a single- or multiple-trap model. We present evidence that may suggest that at least part of pIRIR signal is derived from a high temperature trap (∼550°C thermoluminescence (TL) peak), although again the data can also be explained in terms of a single-trap model. Finally, we present dose response curves and characteristic curvature constants (D₀) values for various IRSL signals and conclude that the more stable signals saturate more quickly than the less stable signals and that the initial and final signals saturate at approximately the same level.     

Rock surface luminescence dating of prehistoric rock art from central Iberia

Rock art paintings are notoriously difficult to date numerically. Recently, luminescence dating has been shown to provide reliable rock surface burial ages in various archaeological settings. Here we use the cross-cutting relationship between a fallen rock and two paintings of the Iberian Levantine (older) and Schematic (younger) styles to constrain the age of the paintings by dating the rockfall event using rock surface luminescence dating. Infrared-stimulated luminescence (IRSL) signals as a function of depth into the buried face of the talus border indicate that the IRSL signal measured at 50°C (IR₅₀) was sufficiently reset to a depth of about 1.6 mm prior to burial. An uncorrected IR₅₀ age of 1.6 ± 0.2 ka was calculated for the rockfall event by dividing the surface equivalent dose (D_e) by the total dose rate. This age was corrected using both conventional and field-to-laboratory saturation approaches to yield indistinguishable ages of 2.7 ± 0.5 and 2.9 ± 0.3 ka, respectively. Since the panel with Schematic art was first available to the artist after the rockfall, we conclude the Schematic rock art at Villar del Humo is younger than ~2.9 ka. The Levantine rock art was painted on a panel constrained by the talus boulder before detachment, and so it is likely to be older than ~2.9 ka.     

Comparison of three K-feldspar luminescence dating methods for Holocene samples

The luminescence dating of the K-feldspar fraction is an alternative way for samples that cannot yield reasonable equivalent dose (D_e) from quartz fraction with very weak luminescence signal. For testing the reliability of the infrared stimulated luminescence (IRSL) dating of K-feldspar, luminescence dating was applied to quartz and K-feldspar fractions respectively for several Holocene samples in this study. K-feldspar apparent ages using routine single aliquot regenerative-dose (SAR) protocol, K-feldspar ages using g value correction method and ages from isochron dating method were compared with quartz ages. It is found that the g value correction method cannot give reliable ages due to the large errors induced during measurements. The isochron dating method is effective to the sample with problematically external dose rate. However, isochron dating may introduce a relatively greater error during grain sizes — D_e curve fitting, therefore this method could obtain low-resolution ages for Holocene samples. Even K-feldspar apparent age from routine SAR protocol is relatively younger by about 10% than the quartz age, it still could establish reasonable chronological framework for Holocene samples.     

Luminescence dating of anthropogenic deposits from Tall Zarʿa in the Jordan Valley

This study uses quartz-based optically stimulated luminescence dating to determine when a massive fortification wall (W11186) was constructed in the archaeological site of Tall Zarʿa in the Jordan Valley. A total of 11 samples of sediments were taken from a trench on the north side of the wall (extramuros). The extracted quartz grains had good luminescence characteristics and were identified as well bleached by comparison with feldspar infrared-stimulated luminescence (IRSL) ages. The optical ages showed that the deposition against the wall occurred in two different periods. The first was around 3.20 ± 0.07 ka ago (Iron Age), and the second was around 2.28 ± 0.08 ka (Hellenistic period). Human activity was evident because of the intermixing of cultural material with the presumed naturally deposited units.     

TL and IRSL dating of Jiahu relics and sediments: clue of 7th millennium BC civilization in central China

Thermoluminescence (TL) dating of pottery and infrared stimulated luminescence (IRSL) dating of sediments from early Neolithic layers at the Jiahu site, Henan Province, east-central China, have been achieved. The pottery TL ages range from 6800 (±450) to 8900 (±640) years and the sediment IRSL ages from 6750 (±760) to 8860 (±870) years confirming former ¹⁴C data. Both TL and IRSL ages agree well with each other. They reinforce the very early existence of a fully developed Neolithic civilization in central China, starting already in the first half of the 7th millennium BC and lasting about 2100 years. From these layers finds of bone flutes and Chinese characters have already been reported [X. Li, G. Harbottle, J. Zhang, C. Wang, The earliest writing? Sign use in the seventh millennium BC at Jiahu, Henan Province, China, Antiquity 77 (2003) 31–44; J. Zhang, G. Harbottle, C. Wang, Z. Kong, Oldest playable musical instruments found at Jiahu early Neolithic site in China, Nature 401 (1999) 366–368.] The Jiahu pottery of the 7th millennium BC belongs to the earliest in China and elsewhere.     

Residual doses and sensitivity change of post IR IRSL signals from potassium feldspar under different bleaching conditions

The residual doses and sensitivity change for potassium-rich feldspar (K-feldspar) have been studied using the post-infrared infrared stimulated luminescence (pIRIR) and multi-elevated-temperature post-IR IRSL (MET-pIRIR) protocols. Laboratory simulated poorly-bleached and well-bleached samples were those K-feldspar grains bleached using a solar simulator for 10 minutes and 8 hours, respectively. The residual doses rise with stimulation temperature and time. The poorly-bleached sample has larger residual doses than the well-bleached sample, especially at high stimulation temperatures. The high-temperature pIRIR signals contain a large amount of hard-to-bleach signals. A decrease of luminescence sensitivity was observed after conducting a high-temperature-treatment in the measurement cycles. The sensitivity decreases significantly between the first and the second cycle. The extent of decrease in sensitivity shows a clear temperature trend. The higher the stimulation temperature of pIRIR signals is, the larger the sensitivity decreases. This decrease is more severe for the poorly-bleached sample than for the well-bleached sample, and could possibly lead to problems in sensitivity correction.     

Lexsyg — A new system for luminescence research

The newly developed lexsyg system by Freiberg Instruments is a versatile luminescence reader, suited for research on the luminescence of materials, fundamental research in luminescence dating, but also for routine mass measurements in retrospective dosimetry as well as in dating application. The 80 sample storage wheel is disconnected from the measurement chamber and therefore crosstalk of optical stimulation is absent and cross-irradiation is negligible from the α- and β-sources, which are providing very uniform irradiations, with the latter especially designed for radiofluores-cence (RF) measurement. Optical excitation sources and filter wheels to vary detection wavelengths can be programmed to change at almost any time within measurement sequences, including the auto-mated change of an optional wheel holding up to four different detectors. Thermoluminescence meas-urements and preheating are possible with a versatile heater, which can be programmed for linear or non-linear heating or cooling, as well as holding a temperature constant. Rates as well as durations can be varied, together with individual ramping, staging and cooling for an almost unlimited number of steps. Violet- and IR-lasers, green and blue LED-arrays can be operated in continuous (CW) or modulated mode (linear/non-linear), and optionally for pulsed as well as time resolved luminescence detection. Six arrays of power LEDs allow the simulation of different bleaching regimes (‘solar simu-lator’), while luminescence detection can be achieved by a variety of photomultiplier tubes and by CCD cameras for spatially resolved measurements and luminescence spectra.     

Comparing different post-IR IRSL approaches for the dating of Holocene coastal foredunes from Ruhnu Island,Estonia

Different post-IR Infrared Stimulated Luminescence (IRSL) approaches are applied to sediments from a Holocene coastal foredune sequence on Ruhnu Island in the eastern Baltic Sea. The comparison of D _e-values and ages determined by the different approaches is complimented by fading and bleaching experiments. The fading experiments imply strong fading of IRSL (50°C) signals and no fading of any of the post-IR IRSL signals, but this is not confirmed by the determined D _e-values. In fact, post-IR IRSL (150°C) D _e-values agree within errors with those calculated for IRSL (50°C). From the bleaching experiments it is inferred that the higher values observed for post-IR IRSL at more elevated stimulation temperatures (225°C/290°C) are likely related to either thermal transfer and/or slow-to-bleach components within the signal. For the dating of the Holocene foredune sequence of Ruhnu Island, the post-IR IRSL (150°C) approach is preferred and these agree with the limited independent age control available from radiocarbon dating. Accordingly, the sequence formed between ca. 7.0 ka and 2.5 ka ago.     

Luminescence dating of young coastal deposits from New Zealand using feldspar

A new measurement protocol has been tested on K-feldspars from Whanganui Inlet and Parengarenga Harbour, New Zealand. A Single Aliquot Regenerative (SAR) dose protocol, using two successive infrared (IR) stimulations (post-IR IR SAR protocol) is setup for these young (<1000 years) coastal sediments. Significant anomalous fading (g _2days =7 %/decade) is observed using the conventional IR signal measured at 50°C. In contrast, the fading rate of the IR signal measured at elevated temperature (150°C) after the IR stimulation at 50°C (a post-IR IR signal) is not significant (g _2days ≤ 1 %/decade). Surprisingly low residual infrared stimulated luminescence (IRSL) signals were observed for a surface sample, suggesting that accurate ages as young as ∼50 years can be obtained for these recent deposits. IRSL ages ranging between 48±6 years and 1050±50 years are obtained from six samples, indicating that sediment accumulation has occurred at the two sites during the last millennia, despite a falling trend in relative sea-level in Whanganui Inlet and a stable relative sea-level at Parengarenga Harbour.     

Luminescence characteristics and dose distributions for quartz and feldspar grains from Mumba rockshelter,Tanzania

Mumba rockshelter is a key archaeological site for the Middle and Later Stone Age occupation of East Africa, but its chronology has remained unresolved. We report the results of a dating study, focussing on the characterisation of the optically stimulated luminescence (OSL) and infrared stimulated luminescence (IRSL) properties of quartz- and potassium-rich feldspar grains. Quartz has previously proven troublesome for dating in East Africa. We identified five general types of quartz grain behaviour, based on the shapes of their OSL decay and dose–response curves. Dose recovery experiments and measurement of the natural samples revealed particular problems with quartz grains that had hyperbolic dose–response curves, low characteristic saturation doses and anomalously large changes in sensitivity between regenerative-dose cycles. The use of pulsed irradiation during measurement and standard and additional quality-assurance criteria during data analysis reduced the number of grains that suffered from these problems. We applied these procedures to individual grains of quartz from eight samples and, using appropriate statistical models, identified post-depositional mixing in three samples. The remaining samples had scattered equivalent-dose distributions typical of quartz grains that had received variable beta dose rates during burial. Stratigraphically consistent OSL ages were obtained for all but the deepest sample. Feldspar ages were estimated for the latter sample and three other samples, using the elevated temperature IRSL signal that exhibited low rates of anomalous fading. Fading-corrected feldspar ages for the latter three samples are consistent with their single-grain quartz ages, but single-grain dating is needed to address problems of post-depositional mixing.     

INFRARED STIMULATED LUMINESCENCE DATING OF ARCHAEOSEDIMENTS

In this study the feasibility of infrared stimulated luminescence (IRSL) for dating loessic colluvial sediments, deposited as a result of human activity, is investigated. It is demonstrated that the ‘IRSL-clock’is reset after a few minutes of daylight exposure even under foggy weather conditions. Samples of independently known age were taken at the Neolithic Bruchsal Aue site in south-west Germany. Different laboratory procedures are tried and a method is suggested (narrow wave-length band in the blue, preheat at 220° C for 5 min) to overcome age underestimates. This laboratory technique yielded archaeologically reasonable ages for colluvial sediments and hollow fillings. The IRSL-ages demonstrate that the deposition of the colluvia is related to soil erosion triggered by human activities, such as wood clearing and agriculture. The successful dating of archaeosediments has a great potential for applications in environmental archaeology as well as in geomorphology and in particular for the reconstruction of man-landscape interactions in central Europe.     

Non-destructive characterization of archeological Cu-based artifacts from the early metallurgy of southern Portugal

In this study, Monte Carlo (MC) simulations combined with energy dispersive X-ray fluorescence (EDXRF) spectroscopy have been used to characterize non-destructively a collection of Cu-based artifacts recovered from two archeological sites in southern Portugal: (a) the Chalcolithic E.T.A.R. site of Vila Nova de Mil Fontes and (b) the Middle Bronze Age site of Quinta do Estácio 6. The metal artifacts show a multilayered structure made up of three distinct layers: (a) brownish carbonate soil-derived crust, (b) green oxidized corrosion patina, and (c) bulk metal. In order to assess the reliability of the EDXRF-based Monte Carlo simulations to reproduce the composition of the alloy substrate in archeological bronze artifacts without the need to previously remove the superficial corrosion and soil derived patinas, EDXRF analysis together with scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDS) was also performed on cleaned and patina-/crust-coated areas of the artifacts. Characterization of the mineralogical composition of the corrosion products in the surface patinas was further determined by means of X-ray diffraction (XRD). Results suggest that the adopted EDXRF/Monte Carlo protocol may represent a safe and fast analytical approach in the quantitative characterization of the bulk chemical composition of Cu-based metal artifacts even in the presence of fairly thick corrosion patinas and/or soil-derived encrustations at the surface of the archeological objects.     

郑韩故城出土战国晚期铁器腐蚀产物分析

为了分析郑韩故城遗址出土战国晚期铁器的锈蚀产物类型,采用X射线衍射和金相显微观察等现代科技手段,对郑韩故城遗址内仓城铸铁遗址出土的13件样品进行综合研究。通过分析比较样品间的锈蚀程度,发现铁质文物的锈蚀机理复杂,成分多样;一些锈蚀产物中出现明显的分层,锈蚀不均;部分铁器中还存在着活性锈蚀物,其保存状态与金相组织有着密切关系。     

Kinetic analysis of thermoluminescence glow curves in feldspar: evidence for a continuous distribution of energies

The thermoluminescence (TL) glow curves from feldspars have been the subject of numerous studies, because of their importance in luminescence dating and dosimetry. This paper presents new experimental TL glow curves in a plagioclase feldspar, measured using the T _max-T _stop technique of glow curve analysis. Kinetic analysis of the experimental results is carried out for a freshly irradiated sample, as well as for a sample which has undergone optical treatment using infrared light for 100 s at 50°C. Application of the initial rise method of analysis indicates that the TL signals from both samples can be characterized by a continuous distribution of energy levels. By subtracting the TL glow curves measured at successive T _stop values, a series of TL glow curves is obtained which are analyzed using the empirical general order kinetics. It is found that all TL glow curves obtained by this subtractive procedure can be described accurately by the same general order parameter b ～1.7. In a second attempt to analyze the same TL glow curves and possibly extract information about the underlying luminescence process, the shape of TL glow curves is analyzed using a recently proposed physical kinetic model which describes localized electronic recombination in donor-acceptor pairs. Within this model, recombination is assumed to take place via the excited state of the donor, and nearest-neighbor recombinations take place within a random distribution of centers. This recent model has been used recently to describe successfully several types of luminescence signals. This paper shows that it is possible to obtain good fits to the experimental data using either one of these two approaches.     

On the intrinsic accuracy and precision of luminescence dating techniques for fired ceramics

Luminescence dating techniques have been used extensively for archaeological and geological samples. Such techniques are based on thermally or optically stimulated signals. This paper presents simulations of several luminescence techniques for equivalent dose (ED) estimation for ceramic materials containing quartz. The simulations are carried out using a recently published comprehensive kinetic model for quartz, consisting of 11 electron and hole traps and centers. The complete sequence of the experimental protocols for several thermoluminescence (TL) and optically stimulated luminescence (OSL) techniques are simulated using the same set of kinetic parameters. The specific simulated protocols are: additive dose TL protocol, predose technique (both additive and multiple activation versions), phototransfer protocol, single aliquot regenerative optically stimulated luminescence (SAR-OSL) protocol, and SAR thermoluminescence protocol (SAR-TL). One hundred random variants of the natural samples were generated by keeping the transition probabilities between energy levels fixed, while allowing simultaneous random variations of the concentrations of the 11 energy levels. The relative intrinsic accuracy and precision of the protocols are simulated by calculating the equivalent dose (ED) within the model, for a given natural burial dose of the sample. The intrinsic accuracy of these techniques is estimated by simulating natural irradiation of the samples with a known burial dose, followed by simulation of the luminescence method used to recover the estimated dose ED. The percent difference between the burial dose and the ED value represents the simulated accuracy of the luminescence technique. The relative intrinsic precision of these techniques is estimated by fitting Gaussian probability functions to the ED values obtained with the 100 model variants. It is found that the various techniques can reproduce natural paleodoses in the range 10 mGy–10 Gy with a typical intrinsic accuracy of +1 to 10%. Techniques based on single aliquot protocols were found in general to be more precise than techniques requiring the use of multiple aliquots. In addition, techniques based on interpolation of experimental data were found to be consistently both more precise and accurate than those based on extrapolation of experimental data.     

重庆忠县洞天堡墓地出土西汉青铜钫的腐蚀研究

为了解重庆洞天堡墓地出土青铜器的保存状况、腐蚀产物种类和埋藏环境特征等,并探索其锈蚀成因,为即将进行的保护修复工作提供科学的依据,利用三维视频显微镜、激光共聚焦拉曼光谱仪和扫描电子显微镜等对重庆忠县洞天堡墓地出土青铜钫残片进行微观形貌观察和锈蚀物结构成分分析,并利用X射线荧光和微生物分析技术对青铜钫附着土壤进行成分和微生物分析。结果表明:该青铜钫锈蚀物含孔雀石、白铅矿、铅钒、磷氯铅矿、砷铅矿和赤铜矿等;外层锈蚀存在磷和氯元素富集现象;土壤中的磷、硫和氯等元素向青铜器迁移,青铜器中铜、锡和铅元素因腐蚀向土壤中流失;附着土富含多种真菌类微生物,促进了磷氯铅矿和砷铅矿的形成。