Characterization of nonlinearities in the dose dependence of thermoluminescence

Nonlinearities often occur in the dose dependence of thermoluminescence (TL). These include sublinearity, usually when there is an approach to saturation in the dose dependence, as well as supralinearity, also termed superlinearity in the literature. Different researchers in the field have viewed the effect of supralinearity/superlinearity from two somewhat different points of view. One point of view has to do with the rate of change with dose of the dose dependence function. The other approach is related more to the applications of TL in dosimetry and archaeological and geological dating, and basically has to do with the correction to be made in extrapolation in cases where supra(super) linearity occurs following an initial linear dose range, or prior to such a linear range. In the present work we propose quantitative methods to characterize these nonlinearities. We suggest the use of two different nonlinearity indices, depending upon how one wishes to describe the nonlinearity. We propose use of the term “supra linearity index”, ƒ(D), in cases where the feature of interest is the deviation from linearity, namely, when the correction in extrapolation is the main issue. We propose the term “superlinearity index”, g(D), in dose ranges where the growth is “more than linear” and when extrapolation is not the main issue. We mathematically define each of these indices and give examples of their use for different dose dependencies.     

Mechanism of formation of nonlinearity in the dose dependence of the thermoluminescence output for anion-defect α-Al2O3 crystals

The mechanism of formation of nonlinearity in the dose dependence of the thermoluminescence output was investigated for anion-defect α-Al₂O₃ single crystals. The experiments revealed a new specific feature: the nonlinearity of the dose dependence of the thermoluminescence output depends on the heating rate of crystals during recording of thermoluminescence. It was established that this effect and other thermoluminescence features studied earlier for anion-defect α-Al₂O₃ crystals are adequately described in the framework of a unified mechanism associated with the interactive interaction of dosimetric and deep traps. Recommendations are given for a decrease in the range of the superlinear portion in the dose dependence of the thermoluminescence output for the crystals under investigation.     

Intrinsic superlinear dose dependence of thermoluminescence and optically stimulated luminescence at high excitation dose rates

Superlinear dose dependence of thermoluminescence (TL) and optically stimulated luminescence (OSL) has been reported for many materials. The theoretical explanation has been ascribed to competition of either traps or recombination centers, during the excitation stage or during the read-out phase. There has been an account in the literature on superlinearity of OSL associated with merely one trapping state and one kind of recombination center. This had to do with the process taking place during the read-out stage, namely the optical stimulation. In the present work, we report on a model of one trapping state and one kind of recombination center which results in a superlinear filling of the center. Thus, one can expect a superlinear dose dependence of the area under the resulting TL glow peak as well as the OSL signal. We follow this situation by writing the simultaneous nonlinear rate equations for the one-trap-one-recombination-center (OTOR) model and study the expected results by numerical simulation consisting of solving the equations with sets of the trapping parameters. We also present analytical results based on simplifying assumptions, and compare the analytical and numerical results. The effect is significant at relatively high dose rates. The main implication is that when one tries to evaluate by TL dosimetry a dose applied at a high rate, calibration of the TL dosimeter using much smaller dose rates may result in inaccurate results.     

低温燃烧合成法制备的氧化铝陶瓷粉体的发光特性

α-Al₂O₃∶C单晶具有优良的热释光特性,被用做热释光剂量计,但α-Al₂O₃∶C晶体剂量计的形状不易加工,生产成本高且碳在晶体中难以掺杂均匀。采用低温燃烧合成法以无水乙醇为溶剂,尿素为染料,硝酸铝为反应物制备少团簇、分散均匀的片状α-Al₂O₃∶C陶瓷粉体。探讨不同点火温度和不同退火温度对其光致发光特性的影响,不同退火温度对热释光特性的影响以及热释光与辐射剂量(90Sr β)的关系。通过分析α-Al₂O₃∶C陶瓷粉体的光致发光光谱得出：α-Al₂O₃∶C陶瓷粉体的发射波长在395 nm附近,点火温度T≤800℃时,点火温度为500 ℃制备的α-Al₂O₃∶C陶瓷粉体的光致发光强度最强;在相同点火温度T=500 ℃下,经不同温度退火制备α-Al₂O₃∶C陶瓷粉体,点火温度为500 ℃制备的α-Al₂O₃∶C陶瓷粉体经1 000 ℃退火后光致发光强度最强。通过分析α-Al₂O₃∶C陶瓷粉体的热释光曲线得出：退火后的α-Al₂O₃∶C陶瓷粉体在200 ℃左右的热释光峰值占主导,900 ℃退火的α-Al₂O₃∶C陶瓷粉体在200 ℃附近的热释光峰值最强;通过峰高法对900 ℃高温退火处理后的α-Al₂O₃∶C陶瓷粉体位于200 ℃左右的热释光峰做剂量响应曲线,可以看出,在1～50 Gy剂量范围内具有良好的热释光剂量线性响应关系,在50～200 Gy剂量范围内出现超线性响应关系。与α-Al₂O₃∶C晶体(1～10 Gy)和多孔Al₂O₃∶C薄膜(1～10 Gy)相比,α-Al₂O₃∶C陶瓷粉体的线性剂量响应范围明显扩大。此研究可为提高氧化铝陶瓷粉体的热释光性能提供思路。     

Polarization of thermoluminescence of various scheelites

The polarization of the thermoluminescence of various scheelite type single crystals being correlated with the thermal decay of intrinsic hole centres has been measured. The crystals show partial z-polarization of the thermoluminescence. The degree of polarization of the glow light increases with increasing compression of the anionic XO^2-₄ complexes in different crystals. A model explaining the results on the basis of the term diagram of a single oxocomplex is presented.     

Phototransferred thermoluminescence in anion-defect α-Al<Subscript>2</Subscript>O<Subscript>3</Subscript> crystals

Thermally stimulated migration of charge carriers from trapping centers responsible for the main thermoluminescence peak at 450 K to a deep trap was experimentally observed in anion-defect α-Al₂O₃ crystals. Optically induced transport of carriers from the deep trap to the main trap was also observed to cause phototransferred thermoluminescence at 450 K. The results obtained experimentally confirm the adequacy of the basic assumptions made in the model of interactive interaction between main and deep traps in the crystals under study, as well as substantiate the method of repeated obtaining of dosimetric data.     

TL properties of anhydrous CaSO4:Tm improvement

CaSO4:Tm is excellent phosphors for dosimetry of ionising radiations due to their high sensitivity, wide dose range (from 10^?6 to 1 Gy), relatively simple trap structure, good chemical, thermal and physical stability and ease of preparation. Since 1968 have been developed new methods of preparing aim to increase the sensitivity and the linearity of the CaSO₄:Tm thermoluminescence. The objective of this work is to obtain single crystals of CaSO₄:Tm under controlled crystal growth conditions, such as temperature, atmosphere and velocity, aiming to improve the TL sensitivity of the crystals and investigate its dosimetric properties in order to evaluate the applicability of this material to dosimetry.     

Features of thermoluminescence in anion-defective alumina single crystals after highdose irradiation

The effect of high-dose irradiation by electron beam with nanosecond duration and by gamma-rays on thermoluminescence (TL) yield of anion-defective dosimetric Al₂O₃:С crystals is studied. It is shown that in a wide dose range up to 10 kGy no significant changes in the TL curve shape and the temperature position of the main dosimetric peak (T = 460 K) are observed. The TL yield of this peak is in saturation in the high-dose range 5–80 kGy. Then anomalous increase in TL yield is registered at the dose growth up to 800 kGy. With that an intensive band appears in the green spectrum region in the photoluminescence spectrum. The role of aggregate defects forming F₂-type centers with the increase of TL yield in Al₂O₃:С crystals under high-dose irradiation is discussed.     

Alkali hallde thermoluminescent dosimeters

Single crystals of KCl: Ca have been studied as thermoluminescent dosimeters for the measurement of X-radiations from Cu and Mo targets in the range of 5 mR to 50000 R. Depending upon the amount of radiations received by these crystals, thermoluminescence peaks at 85°, 35° and 190°C are observed for a heating rate of 40°C/min. The total area under the thermoluminescence curve is observed to be directly proportional to the amount of radiations received by these crystals. The effect of the lag of time between the exposure to radiations and the heating for thermoluminescence has also been studied.     

Defects generated by irradiation with gamma rays in lead doped KCl–KBr mixed single crystals

In this work we report the behavior of solid solutions of lead-doped KCl–KBr mixed single crystals subjected to gamma irradiation. Various composition of KCl_1−xBr_x (x=0.02, 0.35, 0.50, 0.65, 0.85) doped with 20–40 ppm of Pb²⁺ were used and exposed to ionizing radiation. The defect production seems to be correlated with the observed increasing integrated thermoluminescence glow curve as a function of irradiation at high 10 kGy dose as well as in the low 2.2–130 dose Gy range. The analysis shows the potential use of these mixed crystals as radiation detector. The defects generated by irradiation were monitored by the optical absorption spectrum and the thermally stimulated luminescence.     

Restored thermoluminescence in oxide crystals

In this paper, we present the results of a thermoluminescence study on several oxide crystals, including Y₃Al₅O₁₂ (YAG), Y₃Al₅O₁₂:Nd (YAG:Nd), Lu₂SiO₅:Ce (LSO:Ce), Y₂SiO₅:Ce (YSO:Ce), Gd₂SiO₅:Ce (GSO:Ce), PbWO (PWO), and PbWO:La (PWO:La). A phenomenon involving restoration of thermoluminescence (TL) glow peaks is found to occur in some of the crystals investigated; crystals γ-irradiated at room temperature and subsequently stored for some time in the dark at 77 K exhibit TL glow peaks in the range below room temperature. This phenomenon is caused not by a thermally or optically stimulated process, but rather as a by-product of a tunneling process. The intensity of the restored TL glow peaks measured in LSO:Ce crystals is found to be proportional both to the radiation dose and to the storage-time at low temperature. A phenomenological theoretical model is proposed, in which tunneling recombination occurs between deep electron and hole traps accompanied by the simultaneous ejection of an electron to the conduction band; some of these conduction electrons then repopulate shallow traps. An oxygen vacancy with two trapped electrons is assumed to be the deep electron trap in this model. The role of oxygen vacancies is confirmed by heating in air at 1000 °C. This model is applied specifically to LSO:Ce, and several possible candidates are suggested for shallow traps in that material.     

The colouration by 60 Co-gamma rays of NaCl and KCl crystals doped with europium ions

Pure and europium doped NaCl and KCl crystals have been irradiated with 60 Co gamma rays and with ultraviolet light. The dose was 10 v kGy and temperatures during irradiation were ambient and liquid nitrogen. The effects of irradiation are determined using optical absorption and thermoluminescence. The role of the europium dopant is compared for the two materials. Factors investigated include the temperature of irradiation, the concentration of the dopant and the state of impurity aggregation and precipitation. A link is indicated between impurity precipitates and UV stimulated thermoluminescence.     

Decisive role of polydispersity in the relaxation spectrum of saturated hydrocarbons from plasma-induced thermoluminescence data

The method of plasma-induced thermoluminescence for the first time has been used to investigate the molecular mobility in near-surface nanolayers of molecular crystals (paraffins) with different chain lengths. The investigations have been performed using a NanoLuminograph device (PlasmaChem, GmbH, Germany) under conditions excluding the modifying effect of gas discharge plasma emission on the surface structure under study. The origin of charge stabilization sites on the surface of molecular crystals as well as the influence of the chain length of paraffins and the purity of their chemical composition on the thermoluminescence intensity and the shape of the glow curves have been discussed.     

Dosimetric application of green luminescence in irradiated TLD-500 detectors

The spectral and kinetic characteristics of thermoluminescence (TL) for anion-defective α-Al₂O₃ single crystals in the 4.4–2.2 eV range at 300–600 K were studied. Three-dimensional (3D) plots of the luminescence under research for a sample before and after UV irradiation at 623 K for 30 min were analyzed. The increase in the emission response in the 2.4 and 3.7 eV bands for the sample after the photothermal treatment was observed. The dominant contribution of a thermally stimulated process with first-order kinetics in the regularities of the 2.4 eV luminescence was shown. The linearity of the dose dependences for the 2.4 eV TL response in different samples at 10⁻⁵–1 Gy was demonstrated. The advantage of using the green thermoluminescence in the TLD-500 for solid state dosimetry was discussed.     

Thermoluminescence and dosimetric aspects of topaz from Yono Shigar mine in Pakistan

Topaz shows thermoluminescence (TL) on heating after exposure to ionising radiation. A study was carried out to explore the possibility to design and develop a TLD (thermoluminescence dosimeter) from locally occurring topaz. Topaz was collected from a mine in Yono Shigar valley in northern Pakistan. The samples were identified as topaz by neutron irradiation, X-ray diffraction and X-ray fluorescence. The crystals of topaz were cut into chips of dimensions compatible to the commercial TLD readers. The chips were exposed to ⁶⁰Co and/or ¹³⁷Cs gamma irradiators. The investigation features included glow curve, dose and energy responses, sensitivity, fading, reproducibility and mechanical stability. The TL glow curves revealed a stable peak at about 250 °C, whose height rose linearly with increase of irradiation dose. The TL response versus dose (calibration curve) showed the linear behaviour between 10^?2 and 10² Gy. The dose response was independent of gamma energies of ⁶⁰Co and ¹³⁷Cs. The response of topaz chips remained constant within 10% deviation from the initial value after 30 cycles of reuse. The rate of fading of topaz was very fast just after irradiation and slowed after a few days. Mechanical stability of the chips remained constant during handling in all investigation experiments. The topaz from Yono Shigar mine may be recommended as a TLD for gamma dose within 10^?2–10² Gy.     

Specific features of luminescence of radiation-colored α-Al2O3 single crystals

Results of a comparative study on specific features of luminescence of thermochemical and radiation-colored crystals of aluminum oxide have been described. It is shown that crystals containing oxygen vacancies of different origins have identical main optical properties. A vacancy or vacancy-impurity origin of deep traps has been assumed. Some specific features of thermoluminescence (TL), which are common for both types of crystals, such as the dependence of the TL output on the heating rate and the occupancy of deep traps described by the model of interactive trap system, have been established.     

Simulation of sublinear dose dependence of thermoluminescence with the inclusion of the competitive interaction of trapping centers

The sublinearity of dose characteristics of the thermoluminescence has been calculated in terms of the model of competitive interaction of electron and hole trapping centers. It has been found that the sub-linearity is caused by the nonradiative electron recombination with hole deep traps during irradiation and recording of the thermoluminescence upon linear heating of a dosimetric phosphor. It has been shown that the proposed sublinearity mechanism can be used to explain the dose characteristics of the thermoluminescence of anion-defective aluminum oxide.     

The effect of ultrasonic perturbation on F-centers in Kcl: A thermoluminescence study

The effects of high Frequency (HF) progressive ultrasonic wave on the F-centers in KCl single crystals are discussed in this paper. Ultrasonics of 3 MHz and 9 MHz are used in the present investigation to produce strain wave perturbation on the F-centers. The thermoluminescence (TL) glow curves obtained from X-irradiated normal and strain wave exposed KCl single crystals show two peaks. In the TL glow curves recorded from X-irradiation followed by the ultrasonic wave exposure of KCl single crystals result in the shift of these peaks to higher temperature side with an increase in their separation and a change in relative areas. However, no additional peaks were seen. Apart from this the strain wave perturbation was also found to effect trapping parameters.     

Non-monotonic dose dependence of the Ge- and Ti-centres in quartz

The dose response of the Ge- and Ti-centres in quartz is studied over a large dose range. After an initial signal increase in the low dose range, both defects show a pronounced decrease in signal intensities for high doses. The model by Euler and Kahan [1987. Radiation effects and anelastic loss in germanium-doped quartz. Phys. Rev. B 35 (9), 4351–4359], in which the signal drop is explained by an enhanced trapping of holes at the electron trapping site, is critically discussed. A generalization of the model is then developed, following similar considerations by Lawless et al. [2005. A model for non-monotonic dose dependence of thermoluminescence (TL). J. Phys. Condens. Matter 17, 737–753], who explained a signal drop in TL by an enhanced recombination rate with electrons at the recombination centre. Finally, an alternative model for the signal decay is given, based on the competition between single and double electron capture at the electron trapping site. From the critical discussion of the different models it is concluded that the double electron capture mechanism is the most probable effect for the dose response.     

The role of deep traps in luminescence of anion-defective α-Al2O3: C crystals

This paper presents the results of a study of deep traps responsible for thermally stimulated luminescence in single crystals of the anion-defective corundum α-Al₂O₃: C observed at temperatures of about 703, 778, 830, and 903 K. The effect of the filling of these traps by carriers of both signs on the sensitivity to radiation of the main thermoluminescence peak at 450 K, optically stimulated luminescence, and phototransferred thermoluminescence has been investigated. The results obtained are treated in terms of a model involving interactive competition of traps of different depth.