Concerning infrared-stimulated luminescence from K-feldspars: evidence from heating before stimulating

Repeated heating and stimulation by infrared of feldspar samples causes a reduction in the luminescence signal. Two feldspars were investigated, one microcline and one orthoclase. Empirically the fraction of luminescence signal f(n) remaining after the nth cycle of heating and stimulation is given by f(n)=1−a ln(n) for laboratory dosed samples of both microcline and orthoclase feldspars, for heating temperatures of 150°C, 180°C and 220°C, for heating durations per cycle ranging from 20 s to 2400 s and with the study covering 10 cycles of heating and stimulation. Logarithmic decay of luminescence with time has been explained previously, in other contexts, as due either to quantum tunnelling or to a continuous distribution of states being involved but it is shown that these explanations do not fit the present data. The measured data on f(n) were corrected for the loss of luminescence due to infrared stimulation to ensure that this did not account for the differences between the data and the expectations from models; the functional form f(n)=1−a ln(n) remains valid, although with changed values of a. Numerical simulations of systems involving a limited number of trap depths, from 21 down to 3, were investigated and those with 5 or more trap depths were found to be capable of resembling the data. The simulations could not define a unique pattern of trap depths to match the data, but of the patterns investigated the data were best reproduced by a distribution of at least 5 traps in the energy range from 1.18–1.66 eV. These conclusions augment, and are consistent with, existing information on luminescence mechanisms in potassium-feldspars.     

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.     

Thermo-optical properties of optically stimulated luminescence in feldspars

Optically stimulated luminescence processes in feldspars are subject to competing thermal enhancement and quenching processes: this article describes the thermal enhancement effects for orthoclase, albite and plagioclase feldspars. It is demonstrated that certain lattice vibrational modes can be selectively probed at specific optical excitation energies. The results are described in terms of the Bohr hydrogen model of the OSL donor defects.     

The initial rate of loss of luminescence due to infrared stimulation of K-feldspars

Repeated stimulation by infrared of a feldspar sample causes a reduction in the luminescence signal. The initial rate of loss of luminescence due to infrared stimulation is investigated for a microcline and an orthoclase with preheating at 150°C, 180°C and 220°C for times ranging from 20 to 2400 s.     

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.     

Recuperation of infrared stimulated luminescence of feldspars

After bleaching the optically stimulated luminescence (OSL) signal to a low residual level, the signal has been found to increase during subsequent storage or preheating. This effect is well known in quartz as “recuperation of OSL after bleaching” (Aitken, M.J., Smith, B.W., 1988. Optical dating: recuperation after bleaching. Quat. Sci. Rev. 7. 387–393.). A better understanding of recuperation in feldspars could help the dating specialist, because this process might be different from the recuperation observed in quartz. This paper highlights a few examples of a larger study, which cannot be shown here in complete detail. We carried out a recuperation study of infrared-stimulated luminescence (IRSL) of different feldspars from a mineral collection, mainly alkali feldspars and one albite. The samples were irradiated with doses of 200, 1000 and 2500 Gy in a ⁶⁰Co gamma cell. Subsequently, the samples were stored in the dark at room temperature (3 weeks up to 6 months, depending on the applied dose), so that the very intense irradiation-induced phosphorescence can decrease for many orders of magnitude. The emitted OSL was measured through detection filters also used in dating (Schott UG 11, Hoya U 340 for detection of near UV-emissions and Schott BG 39 for detection in the visible range). Recuperation times up to 100 days were used. The recuperated-OSL emissions were measured either with the optical filters mentioned above or with a modified experimental set-up using a variable interference filter with a continuous detection range from 400 to 700 nm. In some feldspars very intense recuperation signals (up to 100% and more of the initial signal) were observed when optical stimulation was performed with IR and broadband detection using the BG 39 or when detection was carried out in the near ultraviolet region. The IRSL emissions at 410 and 560 nm, measured with the interference filter, showed no recuperation despite a clearly detectable first shine-down.     

Time-resolved infrared stimulated luminescence signals in feldspars: Analysis based on exponential and stretched exponential functions

Time-resolved infrared-stimulated luminescence (TR-IRSL) signals from feldspar samples have been the subject of several recent experimental studies. These signals are of importance in the field of luminescence dating, since they exhibit smaller fading effects than the commonly employed continuous-wave infrared signals (CW-IRSL). This paper presents a semi-empirical analysis of TR-IRSL data from feldspar samples, by using a linear combination of exponential and stretched exponential (SE) functions. The best possible estimates of the five parameters in this semi-empirical approach are obtained using five popular commercially available software packages, and by employing a variety of global optimization techniques. The results from all types of software and from the different fitting algorithms were found to be in close agreement with each other, indicating that a global optimum solution has likely been reached during the fitting process. Four complete sets of TR-IRSL data on well-characterized natural feldspars were fitted by using such a linear combination of exponential and SE functions. The dependence of the extracted fitting parameters on the stimulation temperature is discussed within the context of a recently proposed model of luminescence processes in feldspar. Three of the four feldspar samples studied in this paper are K-rich, and these exhibited different behavior at higher stimulation temperatures, than the fourth sample which was a Na-rich feldspar. The new method of analysis proposed in this paper can help isolate mathematically the more thermally stable components, and hence could lead to better dating applications in these materials.     

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.     

Investigations of the green- and infrared-stimulated luminescence using the recuperation effect

We used the recuperation effect (see also “Recuperation of infrared stimulated luminescence of feldspars” in this issue) for investigating the connection between infrared- and greenlight-stimulated luminescence (IRSL and GLSL) of feldspars by performing a “double-bleach recuperation” experiment. A diode system was used for infrared (IR) stimulation, and a filtered-light unit for greenlight (GL) stimulation. Powdered feldspar samples (2 mg each) of known chemical characterisation from a mineral collection were used. After beta-irradiation with 180 Gy and storage in the dark for several weeks feldspar aliquots were bleached down to a residual level of ≈1% of the initial level, first with IR and subsequently with GL. For both stimulations, detection of the stimulated luminescence was carried out in the near ultraviolet region (around 260–360 nm, peaked at 340 nm). Other aliquots were bleached in reverse order (1st GL, 2nd IR). These bleaching sequences were also applied to recuperation measurements after 30 days storage time under controlled room-temperature conditions. Results of these experiments will be presented and a possible interpretation of the observed recuperation signals in terms of a two-trap optically simulated luminescence model will be given. The different interaction of the traps, depending on the specific feldspar, will be shown.     

一种天然正长石的释光特性

应用RGB-3B型热释光仪和BG2003释光谱仪对一种正长石矿物的热释光和选频释光发光曲线进行测定,获得正长石的释光特性。研究表明：天然正长石的三个热释光峰峰温为148,197,310 ℃,辐照一定剂量后,出现197 ℃和263 ℃两个稳定的热释光峰。正长石的峰位温度随着增温速率的减小,向左移动。选频热释光290, 300, 310, 340, 400, 480 nm存在释光响应,选频绿光释光280, 290, 300, 310, 320, 400, 460, 480 nm存在释光响应,400 nm频道的光子计数随剂量的变化具有一定的线性关系,具有辐射剂量计的特性,具备释光测年的应用潜力。     

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.     

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.     

Mechanisms of luminescent responses in thermal and optical stimulation of potassium feldspars

We propose a model describing the mechanism for generation of an optically stimulated luminescence signal in potassium feldspars when irradiated in an IR absorption band (IR OSL). The model assumes that this type of stimulated luminescence is intercenter by nature, arising in tightly bound deep trap/ionized luminescence center pairs. At the same time, the thermoluminescence (TL) signal and the optically stimulated afterglow (OSA) signal arise in a recombination process with participation of the conduction band. We describe the results of an experimental test of the proposed model.     

Comparison of ‘blue’ and ‘infrared’ emission bands in thermoluminescence of alkali feldspars

Dating quaternary sediments by thermoluminescence (TL) or optically stimulated luminescence (OSL) calls for a detailed knowledge of the luminescence of feldspars. TL of the various alkali feldspars ((K, Na) Si₃AlO₈) display many common features, and some of these cause great difficulties for dating. After long storage following ionizing irradiation, the TL of most alkali feldspars is known to fade away by “anomalous fading”, which is incompatible with dating. This effect had been attributed to tunnel recombination. Following irradiation, a very intense tunnelling afterglow is observed at temperatures down to liquid nitrogen, in accordance with the observed rate of fading. This emission has a Gaussian spectrum entirely in the infrared (IR) with a maximum at 1.7 eV. It displays an important thermal quenching from 77 to 300 K. Its intensity is related with the ‘disorder’ of the crystal lattice. At higher temperatures, in TL proper, two emission bands can be separated. One is the well-studied complex visible emission, distributed over the spectral region from UV to orange, but mostly ‘blue’. The other is the ‘infrared’ band already observed at lower temperatures, which is attributed to Fe³⁺ ions. These two bands are clearly separated, with the spectral maxima, respectively, below and above 600 nm. They have also different kinetics, the glow peaks temperatures are different. But these two different bands are also coupled in many ways, they have parallel growth and fading. With ‘disordered’ feldspars, the ‘blue’ emission displays anomalous fading, which is stronger than that of the ‘infrared’. The infrared emission is more stable, which may be interesting for the purpose of dating.     

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.     

Pulsed photostimulated luminescence of alkali feldspars

The use of pulsed photostimulation techniques has a number of practical and conceptual attractions compared with continuous stimulation approaches. Enhanced signal-to-background ratios, opportunities for signal recovery techniques, and ability of detecting luminescence asynchronously and close to stimulation wavelengths are all of practical interest. In addition, it is possible to measure the time-scale and underlying physical processes of the charge transport and luminescence recombination steps following photostimulation. Proximity effects (localized transitions, tunnelling) and re-trapping can be detected directly. Facilities for pulsed photostimulated luminescence measurements using light-emitting diode (LED) arrays, laser diodes and a pulsed dye laser, with time-domain analysis down to 10^-8s have been developed. These facilities are described, together with results from studies of natural and laboratory induced signals from alkali feldspars measured at various times after irradiation. For the first time it has been shown that the recombination dynamics of irradiated feldspars consist of a complex series of continua and line components, presumed to be associated with distinct charge transport processes between traps and recombination sites. Evidence of post-irradiation modification of recombination dynamics is presented for a series of highly irradiated International Atomic Energy Agency (IAEA) F1 feldspar samples, and for a volcanic lava exhibiting gross short-term fading of both thermoluminescence and photostimulated luminescence. This provides direct evidence that fading is associated with short-range processes between trap and centre and, also for the first time, suggests an effective physically based means of detecting and potentially remedying such behaviour in dating studies.     

Post-IR IRSL production in perthitic feldspar

A museum sample of perthitic feldspar was used to study the production of post-IR IRSL signals. It was found that traps responsible for low temperature (∼230 °C) TL peaks play an unexpectedly important role in post-IR IRSL production. During the production of the IRSL signal during low temperature IR stimulation (100 °C), electrons are optically transferred from IRSL traps into these TL traps which have been emptied by the preceding preheat at 320 °C. Subsequent heating to 300 °C causes thermal transfer of these electrons from these traps back into previously emptied IRSL traps which are related to the high temperature TL peaks. IR stimulation of these electrons results in post-IR IRSL. Thus the initial source of the post-IR IRSL signal is the same as the IRSL signal, with a role being played by intermediate traps that give rise to TL signals between 200 and 250 °C, and the final source is similar to that of the IRSL signal. Therefore the post-IR IRSL signal is a by-product of the production of the IRSL signal. It was also found that post-IR IRSL production with high post-IR IR stimulation temperatures (e.g. >230 °C) additionally includes a small contribution from the post-IR isothermal decay of high temperature TL peaks that are not sensitive to IR stimulation at low stimulation temperatures.     

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.     

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.     

Further investigations of tunneling recombination processes in random distributions of defects

The shape of infrared stimulated luminescence signals (IRSL) from feldspars has been the subject of numerous studies in the field of luminescence dating. Specifically linearly modulated IRSL signals (LM-IRSL) are commonly assumed to consist of several first order components corresponding to distinct optical stimulation cross sections. This paper models the shape of LM-IRSL signals using a recently proposed kinetic model, which describes localized electronic recombination in donor–acceptor pairs of luminescent materials. 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. The model has been used previously successfully to describe both thermally and optically stimulated luminescence (TL, OSL). This paper shows that it is possible to obtain approximate solutions for the distribution of donors in the ground state as a function of two variables, time and the distance between donors and acceptors. Approximate expressions are derived for several possible modes of optical and thermal stimulation, namely TL, OSL, linearly modulated OSL (LM-OSL), LM-IRSL and isothermal TL (ITL). Numerical integration of these expressions over the distance variable yields the distribution of remaining donors at any time t during these experimental situations. Examples are given for the derived distributions of donors in each experimental case, and similarities and differences are pointed out. The paper also demonstrates how LM-IRSL signals in feldspars can be analyzed using the model, and what physical information can be extracted from such experimental data. The equations developed in this paper are tested by fitting successfully a series of experimental LM-IRSL data for Na- and K-feldspar samples available in the literature. Finally, it is shown that the equations derived in this paper are a direct generalization of an equation previously derived for the case of ground state tunneling.