Natural IRSL intensities and apparent luminescence ages of single feldspar grains extracted from partially bleached sediments

The single aliquot technique has been applied to single grains of K-feldspar extracted from a well-dated late-glacial marine sediment sample for which standard luminescence dating yielded ages that were in excess of the expected age. Natural infrared-stimulated luminescence (IRSL) intensities as well as single grain palaeodoses show a wide range of values. Most of the bright grains yield equivalent doses largely in excess of the expected palaeodose, considering the depositional age of the sample. The luminescence emitted by the brightest grains would dominate the signal emitted from aliquots containing many grains. This explains the overestimation of ages obtained using standard luminescence techniques for the sample investigated. Palaeodoses obtained from grains that exhibit low IRSL intensities are close to the expected dose. However, the age derived from these grains is lower than the expected age. Anomalous fading is believed to be the main cause for the age underestimation. This study is the first demonstration of the feasibility of dating a sedimentary event using the luminescence of a single mineral grain.     

The fadia method: a new approach in luminescence dating using the analysis of single feldspar grains

The fadia method has been recently introduced in luminescence as one that may potentially resolve the problem of anomalous fading and age shortfalls in IRSL dating of sediments. This method takes advantage of the differential fading rates of single feldspar grains and allows one to extrapolate to zero fading. This paper describes step by step the protocol used in the Montréal laboratory. The application of the method is shown to be hampered by the occurrence of faintly luminescent feldspar minerals, and/or unbleached grains in the dated sediment samples.     

Sources of overdispersion in a K-rich feldspar sample from north-central India: Insights from De,K content and IRSL age distributions for individual grains

Luminescence dating of individual sand-sized grains of quartz is a well-established technique in Quaternary geochronology, but the most ubiquitous mineral on the surface of the Earth—feldspar—has received much less attention at the single-grain level. In this study, we estimated single-grain equivalent dose values and infrared stimulated luminescence (IRSL) ages for K-rich feldspar (KF) grains from a fluvial sample underlying Youngest Toba Tuff (YTT) deposits in north-central India, and compared these ages (corrected for anomalous fading) with those obtained from individual grains of quartz from the same sample. Both minerals have broadly similar single-grain age distributions, but both are greatly overdispersed and most grains have ages substantially younger than the expected age of the YTT deposit (～74 ka). Almost half (45%) of KF grains used for age calculation have fading rates statistically consistent with zero, but the age distribution of these grains is as dispersed as that of the entire population. We obtained a similar distribution of ages calculated for 51 grains using their individually measured internal K contents, which exhibited only minor grain-to-grain variation. Given the lack of dependency of single-grain ages on the measured fading rates and internal K contents, and the overall adequacy of bleaching of grains collected from a sandbar in the modern river channel, we consider the spread in ages is most likely due to mixing, at the time of deposition and after the YTT event, of potentially well-bleached fluvially-transported sediments with older grains derived from slumping of riverbank deposits. Some spread may also be due to natural variations in the IRSL properties of individual KF grains.     

Red luminescence from potassium feldspar for dating applications: a study of some properties relevant for dating

Aspects of the red thermoluminescence (RTL) and IR (833±5 nm) stimulated red (λ_emission=600–750 nm) luminescence (orange-red IRSL) of potassium feldspar from different origins are described. Anomalous fading of RTL (300–500°C) from a selection of potassium feldspar samples was tested. High temperature RTL (300–450°C) exhibits less anomalous fading in comparison to UV luminescence, for the samples under study. The result supports the contention of Zink and Visocekas (1997) that the red TL emission from feldspar does not fade. It was found that RTL is bleachable due to IR exposure, and the relationship between RTL lost and orange-red IRSL produced is linear. It is shown that around one third of the trapped charge responsible for the orange-red IRSL signal gives rise to an RTL signal, indicating that some traps and luminescence centres are shared for RTL and orange-red IRSL.

Specific characteristics of orange-red IRSL from feldspar were identified. It was found that the orange-red IRSL decay curve is bleachable by IR and daylight and can be described by the sum of three exponential components. Orange-red IRSL fading was tested. Short-term storage tests (up to 2 weeks) showed no fading. Longer-term (ca. months) storage of orange-red IRSL do in fact indicate fading, though at levels considerably lower than for the UV emission. The contradictory result is possibly due to the detection wavelength. As such, it is highly likely that the long-term fading experiment is strongly influenced by the feldspar emission centred at ca. 570 nm, which exhibits anomalous fading, while the short-term fading experiment is more greatly influenced by the far red emission centred at ca. 710 nm that in comparison to UV emission shows no or less fading.     

Infrared (IR) stimulated luminescence from modern bricks in retrospective dosimetry applications

It has frequently been observed that certain roof tiles and bricks, especially from relatively modern European buildings, do not contain enough quartz grains in a suitable grain size range to permit dose reconstruction using thermoluminescence (TL) or optically stimulated luminescence (OSL) methods. In this paper the feasibility of using infrared-stimulated luminescence (IRSL) on the feldspar fraction of such bricks and tiles has been investigated. Appropriate preheating treatments were employed in order to select the most stable signals, and procedures were developed to enhance the signal to noise ratio. The possible effect of anomalous fading under application of these procedures was tested. In the dose range above 100 mGy, it has been demonstrated that using IRSL on the feldspar fraction of such material provides a feasible alternative to the use of green-light-stimulated luminescence (GLSL) on the quartz fraction, for the purposes of retrospective dosimetry. Furthermore, since the use of IRSL as described in this paper involves the measurement of polymineral fine grain fractions of bricks, a technique for the calibration of the built-in β source against the γ source in Secondary Standard Dosimetry facilities for routine use of the technique is described.     

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

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

Na-rich feldspar as a luminescence dosimeter in infrared stimulated luminescence (IRSL) dating

One of the challenges in dating rock surfaces is the choice of the luminescence mineral. Although quartz is the preferred dosimeter in sediment dating, it is often not sufficiently sensitive when extracted from solid rocks. The intensity of signals from feldspars tends to be much less dependent on geological origin and erosion history, but the dosimetry of K-rich feldspar grains extracted from rocks is complicated because the internal dose rate is very dependent on the original feldspar grain size. The in situ grain size information is lost during the crushing process used to separate the grains for measurement. This latter problem does not apply to Na-rich feldspar because of the absence of internal radioactivity.The potential application of Na-rich feldspar as a luminescence dosimeter for the IRSL dating of rock surfaces is investigated using a variety of sediment samples from different geological settings for which independent age control is available. The blue and yellow luminescence emissions are measured for IR stimulation at 50 °C (IR₅₀), and post-IR IR stimulation at 290 °C (pIRIR₂₉₀). Thermal stability experiments imply that the corresponding signals in both emissions have comparable thermal stabilities and that all signals have similar recombination kinetics and are thermally stable over geological timescales. The IR₅₀ doses measured using blue and yellow emissions are similar to or lower than quartz doses while pIRIR₂₉₀ blue doses are higher than those from yellow emission and quartz doses. The fading rates measured for the IR₅₀ signals are ∼3%/decade larger than those measured for the pIRIR₂₉₀ signals in both yellow and blue emissions. Furthermore the average fading rates of both yellow signals are ∼3%/decade higher than the corresponding fading rates of the blue signals. However, there is no detectable correlation between fading rates and the measured D_e values. The residual doses measured from the laboratory-bleached samples and a modern analogue suggest that the IR₅₀ signals in both blue and yellow emissions bleach to the same degree, as do the corresponding pIRIR₂₉₀ signals, and that there is no significant naturally-unbleachable residual dose observed using these signals. Neither anomalous fading nor incomplete bleaching explains the observed dose discrepancy between the two emissions. Eight uncorrected and fading-corrected ages are calculated for each sample based on all four signals, using the dose rate relevant to Na-rich feldspar extracts (i.e. ∼3% K). The IR₅₀ and pIRIR₂₉₀ blue ages were also calculated assuming a dose rate based on 12.5% internal K (i.e. assuming that the blue signals were mainly derived from contamination by K-rich feldspar). The latter pIRIR₂₉₀ blue ages are in agreement with the expected age control, raising the possibility that this signal originates mainly from K-rich feldspar contamination in our Na-rich fractions, and thus is not so useful in the luminescence dating of rock surfaces. On the other hand, the pIRIR₂₉₀ fading-corrected ages based on the yellow emission are consistent with the independent age controls; higher preheat and stimulation temperatures may result in more stable yellow signals from Na-rich feldspar extracts from rocks, and so reduce the size of the fading correction. We conclude that, because this signal avoids the dosimetry difficulties of K-rich feldspar extracts, it has considerable potential in the IRSL dating of rock surfaces.     

Testing Post-IR IRSL protocols for minimising fading in feldspars,using Alaskan loess with independent chronological control

Concern over anomalous fading has been the biggest single factor responsible for deterring the widespread use of the infra-red stimulated luminescence (IRSL) or thermoluminescence (TL) signal from feldspars for luminescence dating. There has therefore been great interest in the use of the recently proposed Post-IR IRSL signal, because it has been shown to significantly reduce the degree of anomalous fading observed in feldspars and therefore potentially provides a means of circumventing the issue. This study undertakes a systematic investigation into various preheat and Post-IR IRSL measurement conditions proposed in the literature, by using two samples from the Halfway House loess section in Alaska which bracket the Old Crow tephra which has been dated using fission track methods. Preheat plateau tests show a dramatic change in equivalent dose with Post-IR IRSL measurement conditions, and further tests reveal that these changes are driven by preheat temperature rather than Post-IR IR stimulation temperature. Dose recovery tests on laboratory-bleached material mimic the findings of the natural preheat plateau test data, and sensitivity change between the first and second Single Aliquot Regenerative dose (SAR) measurement cycle is found to be responsible. Comparison of the Post-IR IRSL ages with the independent age control shows that, for the samples in this study, the Post-IR IR signal stimulated at 290 °C is inappropriate for dating. However, use of lower preheat (250–300 °C) and Post-IR IR stimulation temperatures from 225 to 270 °C gave rise to ages which were in agreement with the independent age control.     

Determining the K-content of single-grains of feldspar for luminescence dating

Feldspars form a solid-solution series whereby the K-content may range from 0 to 14%. LA-ICP-MS measurements for density-separated single-grains of feldspar yielded realistic concentrations of K within the range of those naturally occurring, and also highlighted the difficulty in isolating the pure end members during density-separation. No direct relationship was found between the thermal stability of the infrared-stimulated luminescence (IRSL) signal and measured K-content of individual grains. However, the brightest IRSL and post-IR IRSL signals originated from grains with ～12% K-content. All grains giving a measurable signal had K-content between 6 and 13%, therefore it is suggested that an internal K-content of 10 ± 2% can be assumed for routine single-grain dating of density-separated K-feldspars.     

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.     

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.     

Luminescence properties of biotite relevant to dating and dosimetry

Biotite mineral grains from granitic rocks were subjected to luminescence studies with optical and thermal stimulation. Moderate thermoluminescence (TL) signals and weak optically stimulated luminescence (OSL) with blue-green light stimulation were detected after 50 Gy beta irradiation. No detectable infrared-stimulated luminescence (IRSL) was observed for natural and laboratory beta-irradiated samples. TL peaks at 118, 300, 360 and 480 °C can be identified from laboratory-irradiated samples. The 360 °C TL peak saturates at a higher dose than quartz, but shows significant anomalous fading after 80 days stored at room temperature. The potentials and problems for biotite used as a natural dosimeter are discussed.     

Investigating the contribution of recuperated TL to post-IR IRSL signals in a perthitic feldspar

Using a museum specimen of perthitic feldspar, the characteristics of post-IR IRSL production at 200 °C after different prior IR bleaching at 100 °C were investigated. It was found that the post-IR IRSL signal had an isothermal TL contribution that was unexpected following a previous preheat at 320 °C; this is the result of isothermal decay of recuperated TL peaks resulting from photo-transfer that occurred when the previous IRSL signal was measured at a lower temperature. The isothermal TL contribution to the post-IR IRSL signal depends on prior IR bleaching conditions. Since the recuperated TL signal comes from photo-transfer during IRSL production, this signal should also suffer from anomalous fading. Thus, it is suggested that this isothermal TL contribution to the measured post-IR IRSL is removed by the inclusion of an additional step, a cut-heat to 300 °C, in the post-IR IRSL dating protocol.     

A comparative study of the luminescence characteristics of polymineral fine grains and coarse-grained K- and Na-rich feldspars

The IRSL and post-IR IRSL (pIRIR) signal characteristics of polymineral fine grains are investigated and compared with those of K- and Na-rich feldspar extracts. TL signal loss after IR and pIRIR stimulations occurs mainly at around 320 °C for polymineral and Na-feldspar samples and around 410 °C for K-feldspar samples, when a preheat temperature of 250 °C for 60 s is used. After preheating to a higher temperature (320 °C for 60 s) all samples show a TL reduction around 410 °C in the blue detection window. Pulse annealing experiments for IRSL and pIRIR signals for preheats between 320 °C and 500 °C indicate that the signal stabilities are similar among the different feldspar types, when a higher preheat temperature (>320 °C) is used. Thermal activation energies for IRSL and pIRIR signals are largest in K-feldspar and smallest in polymineral fine grains, in both blue and UV detection windows for both fast time-resolved (TR) and continuous wave (CW) signals. These results suggest that IRSL and pIRIR signals in polymineral fine grains originate mainly from Na-feldspar grains; these signals are less thermally stable than those from K-feldspar, but a more stable signal (presumably from K-feldspar grains) can be obtained using a higher preheat temperature.     

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).     

Optically stimulated phosphorescence in orthoclase feldspar over the millisecond to second time scale

In the past, time-resolved IR stimulated luminescence (TR-IRSL) curves from feldspar have mainly been measured over a few hundred μs with the purpose of estimating the lifetimes of the components. In this study, we present the decay form of time-resolved IRSL and IR stimulated phosphorescence (IRSP) from orthoclase feldspar covering over 8 orders of magnitude (50 ns to ～7 s). A detailed characterisation of the slowly decaying signals (ms to s time scales) from feldspar is undertaken to obtain further insight into the role of re-trapping in both the IR stimulated luminescence (IRSL) and the relatively more stable post-IR IRSL signals. The decay form of the different signals examined here shows a weak dependence on preheat temperature and a strong dependence on stimulation temperature. Interestingly, the IRSP curves show a conspicuous kink of which the position is linearly dependent on the on-time duration.The data on thermal dependence of these signals might suggest that the decay behaviour of the time-resolved IRSL and phosphorescence signals mainly reflect the occupancy of electrons in the band tail states with a significant contribution from the shallow traps. This interpretation is supported by thermoluminescence (TL) curves showing the photo-transfer effect during short IR and post-IR IR stimulations.     

The relationship between thermal activation energy,infrared stimulated luminescence and anomalous fading of K-feldspars

A strong dependence of thermal activation energy (TAE) on infrared (IR) stimulation time for the infrared stimulated luminescence (IRSL) signal was observed for K-feldspar grains extracted from several sediments and granites from China. A TAE value as low as ～0.1 eV was observed at the beginning of IR stimulation and increased to ～0.45 eV after 90 s. For a trap depth of ～2 eV below the conduction band for the IRSL traps, the TAE value of ～0.45 eV is consistent with the energy gap between the excited states (～0.5 eV below the conduction band) and conduction band. This phenomenon is explained as the result of the coexistence of thermally assisted recombination via conduction band or band-tail states hopping and athermal tunnelling recombination of electrons from the excited states under IR stimulation, leading to the observation of a higher anomalous fading rate in the initial part of the IRSL decay curve.     

Luminescence sensitivity changes of polymineral fine grains during IRSL and [post-IR] OSL measurements

Sensitivity changes during measurement sequences of infra-red-stimulated luminescence (IRSL) and post-IR optically stimulated luminescence (OSL) are presented for a sample of loess from northwestern China. Together with a dose recovery experiment, the results are used to investigate the ratio of 2.4 found for the D_e values (for IRSL and [post-IR] OSL) obtained when using a single-aliquot regenerative-dose (SAR) protocol in which both D_e values are obtained in a single sequence of measurements. Responses to test doses for both the IRSL and [post-IR] OSL show progressive luminescence sensitivity changes with repeated measurement cycles, with a slight dose dependence for the IRSL. In addition, five modified SAR procedures were used, varying preheats, filter combinations and method of measuring the luminescence signal. The D_e values for all IRSL measurements were at least 50% greater than those for the [post-IR] OSL signal. A modified SAR sequence was also applied in which 0.1 s stimulations (using both IR and blue light sources) were made between all sample treatments. A lack of consistency in the measured luminescence sensitivity of the natural IRSL signal suggests that the [post-IR] OSL signal provides the more reliable value of D_e.     

Limits to depletion of blue-green light stimulated luminescence in feldspars: implications for quartz dating

Feldspar contaminants in quartz aliquots, either as micro-inclusions or as remnant grains (due to inadequate etching) can affect the accuracy and precision of paleodose estimates based on blue-green light stimulated luminescence (BGSL). Such contamination could also alter the shape of the BGSL stimulation curve of otherwise pure quartz. In this study, the functional relationship between the infra-red stimulated luminescence (IRSL) and BGSL of feldspars, (1) at different preheats, and (2) with IR bleaching at different stimulation temperatures and durations, is examined. The results suggest two trap populations participate in the feldspar BGSL process. These are: (1) Type (A) trap populations that can be stimulated by both the infra-red and the blue-green light at 125°C and, (2) Type (B) trap populations that respond only to blue-green-light stimulation at 125°C. However, infra-red stimulation at elevated temperature (220°C) (ETIR) permits depletions of charges in Type (A) and Type (B) to the extent that the feldspar BGSL can be reduced by up to 97% in 5 min.

These results offer prospects for (1) improved precision in paleodose estimates based on quartz; (2) BGSL dating of quartz in a polyminerallic fine grain samples; (3) age estimates based on both quartz and feldspars from the same aliquots, and (4) dating based on feldspar micro-inclusions.     

Study of the relationship between infrared stimulated luminescence and blue light stimulated luminescence for potassium-feldspar from sediments

In luminescence measurements of potassium-feldspar (K-feldspar), both infrared (IR) and blue light (BL) can be used as stimulation sources. Component analysis suggests that the blue light stimulated luminescence (BLSL) measured at 60 °C from K-feldspar can be fitted using three components, namely fast, medium and slow. In order to explore the relationship between the origin of the infrared stimulated luminescence (IRSL) signal and the different components of the BLSL, five sets of experiments were conducted, namely post-IR BLSL (pIR-BLSL), post-BL IRSL (pBL-IRSL), pulse annealing tests, dose response and laboratory fading rate tests. It is observed that most of the IRSL signal can be bleached by BL, while the BLSL signal can only be partially bleached by the IR. The sources for IRSL are mainly associated with the fast and medium components of the BLSL signal.