Variations in luminescence properties of single quartz grains and their consequences for equivalent dose estimation

In this paper examples of variability of luminescence properties between single grains of quartz extracted from natural samples or from crushed single crystals are shown. It is demonstrated how measurements of glow curves, PSL (photon stimulated luminescence) decay curves, thermal activation characteristics using multi-grain aliquots can lead to a misinterpretation of the obtained data. The possible consequences for different D_E estimation techniques applied to multi-grain aliquots or to single grains and normalisation techniques applied to multi-grain aliquots are discussed. In particular pre-dose, multi-aliquot additive, and single grain PSL SAR D_E estimation methods are considered.     

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.     

Radioluminescent dosimetry of α-quartz

The variation in the ultraviolet component of the radioluminescence intensity during X-ray excitation of α-quartz has been found to be dependent on the dose of previous ionizing irradiation. A new method of radiation dosimetry using UV radioluminescence is described. Radioluminescent dosimetry measurements of γ-rays produced by Chernobyl accident and background irradiation were made using natural and extracted crystalline quartz.     

Characterisation of a real-time fibre-coupled beryllium oxide (BeO) luminescence dosimeter in X-ray beams

For the first time the feasibility of using beryllium oxide (BeO) ceramics as a fibre-coupled radioluminescent dosimeter is investigated. BeO ceramic exhibits both radioluminescence (RL) and optically stimulated luminescence (OSL), and has the potential to be a near tissue equivalent alternative to Al₂O₃:C. A BeO fibre-coupled radioluminescence dosimeter is demonstrated and characterised for 6 MV X-rays and superficial X-ray energies, 150 kVp and 120 kVp. Based on the results, we demonstrate the capability of the RL BeO FOD for accurate and reproducible dose measurements with a linear dose rate and dose response. It has also been found that the percentage depth dose curves for 6 MV agreed with ion chamber measurements to within 2%, except in the build up region. For the 150 kVp and 120 kVp photon beams, the depth dose measurements agreed with ion chamber measurements to within 2.5% and 4%, respectively.     

Radioluminescence of LiF:Mg,Ti induced by 4 MeV electrons

This paper reports on the radioluminescence characteristics of LiF:Mg,Ti induced by 4 MeV linear accelerator electrons. The main emission peak of the luminescence is found at 410 nm, but weaker emission occurs around 320, 360, 460, 520 and 560 nm as well. The relative intensities of the emission bands show a strong dependence on the Mg concentration of the sample. The radioluminescence signal reaches its maximum typically 1.5 ms after the irradiation pulse, and decays with a half-life of 4–6 ms. Both the build-up time and the half-life decreases with increasing Mg concentration. The luminescence yield shows a strong dependence on the irradiation dose.     

The basic principle of radioluminescence dating and a localized transition model

The IR signal of the radioluminescence of potassium feldspars is caused by the luminescent transition of electrons into optically active traps. This allows the direct determination of the density of trapped electrons and therefore a method of sediment dating with higher precision and accuracy than conventional luminescence dating. The principle behind it and its advantages are presented, in particular the fact that it is a real single aliquot dating technique. The explanation of both radioluminescence and IR-optically stimulated luminescence (IR-OSL) in terms of a band model is possible after the introduction of a localized transition. In contrast to previous models, the process of dose accumulation in the sediment was simulated using a dose rate as low as in real sediments. Preheat experiments indicate that the recombination centres are the unstable part of the luminescence process. The parameters of these centres are equal to those previously assigned to thermally unstable electron traps. Furthermore, the sources of systematic errors in conventional IR-OSL dating are discussed.     

Real time dose rate measurements with fiber optic probes based on the RL and OSL of beryllium oxide

This work covers the examination of fiber optical probes based on the radioluminescence and real time optically stimulated luminescence of beryllium oxide. Experiments are carried out to determine the fundamental dosimetric and temporal properties of the system and evaluate its suitability for dose rate measurements in brachytherapy and other applications using non-pulsed radiation fields. For this purpose the responses of the radioluminescence and optically stimulated luminescence signal have been investigated in the dose rate range of 20 mGy/h to 3.6 Gy/h and for doses of 1 mGy up to 6 Gy. Furthermore, a new, efficient analysis procedure, the double phase reference summing, is introduced, leading to a real time optically stimulated luminescence signal. This method allows a complete compensation of the stem effect during the measurement. In contrast to previous works, the stimulation of the 1 mm cylindrical beryllium oxide detectors is performed with a symmetric function during irradiation. The investigated dose rates range from 0.3 to 3.6 Gy/h. The real time optically stimulated luminescence signal of beryllium oxide shows a dependency on both the dose rate and the applied dose. To overcome the problem of dose dependency, further experiments using higher stimulation intensities have to follow.     

Radioluminescence (RL) behaviour of Al2O3:C-potential for dosimetric applications

The radioluminescence (RL) of carbon doped aluminium oxide (Al₂O₃:C) TL dosimeter material (TLD-500) was investigated using a ¹³⁷Cs conversion electron source (which also emits β and γ) for simultaneous irradiation and luminescence excitation. Furthermore, RL dosimetry characteristics of this material were studied. The main RL emission occurs at 420 nm. That matches the known main TL and OSL emissions for this material as well as an emission that was investigated in earlier RL studies, excited at higher energies (4 MeV electrons) and very high pulse delivered doses (≈800 kGy·s⁻¹). Furthermore, the saturation dose for the main peak is reached at the dose level of ≈80 Gy as known from TL and earlier RL investigations. Other peaks at 700 and 790 nm and broad emission bands at photon energies higher than 3.00 eV and others between 2.00 and 2.50 eV were observed. The 700 nm emission shows growth also at higher dose levels, and saturates at an estimated dose of ≈800 Gy. The 790 nm emission reaches its maximum intensity at ≈10 Gy absorbed dose. The reported results give an outlook to the usability and the potential of Al₂O₃:C combined with RL measurements for radiation dosimetry as well as for beta source calibration, using radioluminescence.     

Dose rate measurements with a ruby-based fiber optic radioluminescent probe

Fiber optic radioluminescence dosimetry allows real-time dose rate measurements in complex, narrow geometries and at places of high dose rates, without exposing the operator or the susceptible electronics. The keys are the spatial separation of radiation sensitive probe and electronic processing system and their optical connection by a flexible light guide. The small probes are capable of measuring fields of high dose rate gradients and the sealed probe-tip qualifies for applications in the fluid milieu and even for in-vivo-dosimetry. One problem of fiber optic dosimetry is the generation of Cherenkov radiation and fiber luminescence in the irradiated light guide, the so called stem effect. Ruby (Al₂O₃:Cr) has a narrow radioluminescent emission at 694 nm and is a potential luminophor for fiber optic radioluminescence dosimetry. In this work the influence of the stem effect on our ruby-based fiber optic dosimetry system is examined. The behavior of ruby probes under irradiation up to 0.5 kGy, as well as their luminescence decay characteristics and the applicability for measurements in radiotherapeutic fields are investigated.     

Testing the accuracy of a Bayesian central-dose model for single-grain OSL,using known-age samples

While reviews of comparisons between multi-grain OSL ages and independent chronological information are available in the literature, there is hardly any such performance test for single-grain OSL ages. And yet, this is all the more needed as the interpretation of single-grain dose distributions remains a difficult task, given the typically considerable dispersion in equivalent dose values measured by OSL – and the numerous sources of such dispersion in measurements. Here, we present the study of 19 samples for which independent age control is available, and whose ages range from 2 to 46 ka. Based on multi-grain OSL age estimates, these samples are presumed to have been both well-bleached at burial, and unaffected by mixing after deposition. Two ways of estimating single-grain ages are then compared: the standard approach on the one hand, consisting of applying the Central Age Model to D_e values determined with the Analyst software; on the other hand, the central dose model recently proposed by Combès et al. (Combès, B., Philippe, A., Lanos, P., Mercier, N., Tribolo, C., Guerin, G., Guibert, P., Lahaye, C., in press. Quaternary Geochronology). The median of the relative discrepancy between single-grain OSL and reference ages is about twice as large for the standard approach (12%) as with the Bayesian model (7%). Statistical tests show that, based on our (limited) dataset, the difference between the two models seems to be significant for samples in the age range 4–46 ka. Finally, the influence of various factors on the (in-)accuracy of single grain OSL ages is discussed; it appears that the accuracy of ages estimated in a standard way decreases when age is increased, while the Bayesian model seems more robust. This study also shows that (i) there is no 20% limit on the CAM overdispersion parameter for well-bleached samples; (ii) dose recovery experiments do not seem to be a very reliable tool to estimate the accuracy of a SAR measurement protocol for age determination.     

On the lattice defects in Nasicon compounds

Summary  Samples of Nasicon compounds (Na super ionic conductor) with different silicon and phosphorus contents were investigated by performing radioluminescence experiments. In all samples examined, the Frenkel pairs, originated by the displacements of sodium ions in lacunar sites, were found to be the dominant defects. Some useful information on sodium ion mobility was obtained from the analysis of radioluminescence spectra.     

多晶凝固及后续调幅分解过程的晶体相场法模拟

采用晶体相场模型,模拟了二元合金多晶凝固及后续调幅分解全过程.结果表明,晶体相场模型可完整再现包括形核、生长、粗化、晶界形成等多晶生长过程以及圆满完成从凝固到调幅分解的多相变过程. 关键词： 晶体相场模型 多晶凝固 调幅分解 组织演化     

Fiber-optic-coupled RbMgF3:Eu for remote radiation dosimetry

A portable fiber optic dosimeter has been developed that incorporates RbMgF₃:Eu²⁺ at the end of a multimode polymer fiber. It uses two stimulation sources and takes advantage of the range of stimulable traps in this compound. We observe radioluminescence (RL) during gamma ray irradiation and show that the low-dose RL increases linearly with increasing dose rate where the minimum detectible dose rate is ∼0.015 μSv/s. We show that pulsed infrared-stimulated (940 nm) optically stimulated luminescence (OSL) can be used for real time dose monitoring. The cumulative dose can be readout after irradiation where a linear OSL dose response was observed when stimulating at 505 nm and the minimum detectable dose is ∼50 μSv.     

Neutron detection with LiCaAlF6 scintillator doped with 3d-transition metal ions

Capability of thermal neutron detection was examined for LiCaAlF₆ (LiCAF) scintillators doped with 3d-transition metal ions. Their radioluminescence spectra were measured with an 241-Am source to simulate ⁶Li(n, α)³H reaction. The sufficiently intense radioluminescence was observed for the Mn, Co and Cu dopants, while only a weak one was observed for Ti, V, Fe and Ni. A Mn doped LiCAF crystal, which showed the highest radioluminescence intensity, was coupled with a Si avalanche photodiode for the examination of its neutron response. It was confirmed that the average current of the photodiode clearly increased under excitation with 13.5 meV neutron flux.     

A new irradiated quartz for beta source calibration

For luminescence dating to be an accurate absolute dating technique it is very important that we are able to deliver absolutely known radiation doses in the laboratory. This is normally done using a radiation source (alpha, beta, X-ray) calibrated against an absolutely known reference source. Many laboratories have used the various different batches of Risø calibration quartz for the calibration of beta and X-ray sources, but these have been largely undescribed. Here we describe in detail the preparation and luminescence characteristics of a new quartz standard, based on a North Sea beach sand collected from south-western Denmark (Rømø). Two grain sizes (4–11 μm and 180–250 μm) have been examined in detail. These were pre-treated (annealed, dosed and annealed again) to sensitise and stabilise the luminescence signals before being given an absolutely known gamma dose from a point ¹³⁷Cs source in scatter-free geometry. The luminescence characteristics are described; the very intense blue-light stimulated signal is dominated by the fast OSL component and the IR-stimulated signal is negligible. The material is shown to be suitable for measurement using SAR, and the dose recovery ratio is indistinguishable from unity with a standard deviation of <2% for multi-grain aliquots. The material is also shown to be suitable for single-grain calibration, with >80% of the grains giving a useful signal. Although there is an unexplained dispersion in our calibration data of ∼3% (which we cannot attribute to instrument variability), we nevertheless conclude that this material is very suitable for transferring absolute known doses from a standardised gamma source to in-built irradiation sources.     

Intraband radioluminescence of LiF crystals

Spectra of high-energy electrons are calculated in the electron-hole ionization-passive region of lithium fluoride crystals for the conditions of intense irradiation by short pulses of accelerated electrons. The yield of intraband radioluminescence of these crystals is estimated in comparison with the yield of this kind of luminescence of more extensively studied NaCl crystals. The calculations demonstrate that the yield of radioluminescence determined by electron transitions in the conduction band of LiF crystals is two orders of magnitude weaker than the yield of analogous luminescence of NaCl crystals. This is explained, first, by special features of the energy band structure and, second, by the form of the energy dependence of the density of states in the conduction band of LiF crystals. The yield of hole-type intraband radioluminescence is estimated for various assumed relations between the widths of the valence and the forbidden bands.     

A spectral radioluminescence study for dating and dosimetry

The spectral distribution of radioluminescence (RL) and its dose dependence was investigated on various substances to get information about the applicability in dosimetry and dating. The list comprises archaeometallurgical slag components (quartz relicts, glassy fraction), bone, cooking salt, corals, egg shell, flint, mussel shell, natural gypsum, natural halite, quartz (sediments, vein quartz) and sugar. The different emission wave-bands and basic features of their RL-dose-characteristics are reported for 18 different samples. Furthermore results of some materials are discussed in more detail.     

Sources of uncertainties in OSL dating of archaeological mortars: The case study of the Roman amphitheatre “Palais-Gallien” in Bordeaux

Archaeological mortars are more convenient and much more representative for the chronology of buildings than brick or wood constructions that can be re-used from older buildings. Before dating unknown samples of mortars, further investigation of OSL from mortars is required and the most efficient methodology needs to be established. In this study we compared the ages obtained by OSL dating of quartz extracted from mortars of the Roman amphitheatre Palais-Gallien in Bordeaux with independent age information.Resetting of the OSL signal occurred during the preparation of mortar when grains of sand (quartz) were extracted and mixed with lime and water. The mortar was subsequently hidden from light by embedding within the structure which is the event to be dated.Various factors contribute to uncertainties in the age determination. The frequency of measured equivalent doses reveals a large scattering. Optical bleaching of certain grains can be partial due to the short duration of the exposure to light. We worked with the single grain technique in order to find and select the grains that were sufficiently exposed to daylight. To determine the average equivalent dose, we tried three different approaches: a calculation of an arithmetic mean and one following either the central age model or the 3-parameter minimum age model, the latter turned out to be the only relevant way to evaluate the experimental data. The proportion of grains included in the calculation of the average equivalent dose represents 2.7–4.7 % of the overall analysed grains. The results obtained for the three out of four samples are approaching the expected age, however, the minimum doses and the corresponding ages are significantly over-estimated in case of two samples.The studied material is very coarse, which causes heterogeneity of irradiation at the single grain scale, and contributes to a dispersion of equivalent doses. Different analytical methods (scanning electron microscopy with energy dispersive X-ray spectroscopy cartography, Beta-radiography imaging, inductively coupled plasma mass spectrometry) were employed to demonstrate the presence of this phenomenon.Despite the extremely large proportion of high equivalent doses in equivalent dose distributions, there is an apparent presence of well-bleached grains at the beginning of equivalent dose distributions. The study shows the potential of dating mortars by single grain OSL.     

BaHfO3:Ce sintered ceramic scintillators

Raw powders of BaHfO₃:Ce were prepared with modified Pechini process and were calcined in the 650–1700 °C range of temperatures, at different atmospheres – air, vacuum and nitrogen–hydrogen mixture. The powders were converted into sintered ceramics by vacuum sintering. The materials were characterized by XRD, TEM, photoluminescence and radioluminescence spectroscopy. UV-VUV excitation spectra were recorded using synchrotron radiation. Excitation spectra proved that atmosphere of preparation significantly influences the host-to-activator energy transfer, which is the most efficient for materials made in reducing conditions. Also radioluminescence efficacy was found to be superior for materials prepared in such conditions.     

Recombination luminescence in lead tungstate scintillating crystals

Room temperature radioluminescence and photoluminescence decay kinetics measurements of Ba-doped PbWO₄ crystals were compared with those of undoped and Mo-doped samples. Photoluminescence decay measurements focus on the coexistence of the immediate (fast) decay having a decay time of a few nanoseconds with slower delayed recombination decay processes. The radioluminescence emission peaking at 500 nm in Ba-doped crystals is similar to that observed in Mo-doped samples. However, photoluminescence of the Ba-doped crystals shows much faster decay kinetics with respect to that of PbWO₄:Mo. Wavelength-resolved thermally stimulated luminescence data (10–300 K) provides complementary information about trapping states and is correlated to photoluminescence decay kinetics.