Monte Carlo simulations of luminescence processes under quasi-equilibrium (QE) conditions

Previous researchers have carried out Monte Carlo simulations of thermoluminescence (TL) phenomena by considering the allowed transitions of charge carriers between the conduction band, electron traps and recombination centers. Such simulations have demonstrated successfully the effect of trap clustering on the kinetics of charge carriers in a solid, and showed that trap clustering can significantly change the observed luminescence properties. While such Monte Carlo simulations have been carried out for TL, there has been no such trap clustering studies for optically stimulated luminescence phenomena (OSL). This paper presents a simplified method of carrying out Monte Carlo simulations for TL and linearly modulated optically stimulated luminescence (LM-OSL) phenomena, based on the General One Trap (GOT) model, which is a special case of the one trap one recombination center model (OTOR) when quasi-equilibrium conditions (QE) hold. The simulated results show that the presence of small clusters consisting of a few traps in a solid can lead to multiple peaks in both the TL and LM-OSL signals. The effects of retrapping and degree of trap filling are simulated for such multi-peak luminescence signals, and insight is obtained into the mechanism producing these peaks. The method presented in this paper can be easily generalized for other types of luminescence solids in which the recombination probability varies with time.     

Superlinear dose response of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals in luminescence materials: An analytical approach

The phenomenon of superlinear dose response of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals has been reported for several important dosimetric materials. We develop new analytical equations for the filling of traps and centers during irradiation and for the read-out stage of annealed luminescence materials, within the context of a two-trap and two-center model. The equations are applicable for both TL and OSL signals in annealed dosimetric materials, and are derived under the assumptions of low irradiation doses and dominant strong retrapping (weak recombination) processes. For low doses all traps and centers display linear dose response, which leads to quadratic dose response of the integrated TL/OSL signals. A new analytical expression is presented for this well-known quadratic dose dependence, in terms of the kinetic parameters in the model. The effect of elevated irradiation temperature on the integrated TL/OSL signals is also considered, and analytical expressions are obtained for this situation as well. A new type of dose-rate effect is reported based on the modeling results, which is due to irradiation during elevated temperatures. The accuracy of the analytical expressions is verified by comparing with the results of numerical simulations.     

An algorithm for unified analysis on the thermoluminescence glow curve

An algorithm was developed to integrally handle excitation by radiation, relaxation and luminescence by thermal or optical stimulation in thermoluminescence (TL) and optically stimulated luminescence (OSL) processes. This algorithm reflects the mutual interaction between traps through a conduction band. Electrons and holes are created by radiation in the beginning, and these electrons move to the trap through the conduction band. These holes move to the recombination center through a valence band. The ratio of the electrons allocated to each trap differs with the recombination probability and these values also relevant to the process of luminescence. Accordingly, the glow curve can be interpreted by taking the rate of electron–hole pairs created by ionizing radiation as a unique initial condition. This method differs from the conventional method of interpreting the measured glow curve with the initial electron concentration allocated to each trap at the end of irradiation. A program using the Visual Studio's C# subsystem was made to realize such a developed algorithm. To verify this algorithm it was applied to LiF:Mg,Cu,Si. The TL glow curve was deconvoluted with a model of five traps, one deep trap and one recombination center (RC).     

Dependence of the anomalous fading of the TL and blue-OSL of fluorapatite on the occupancy of the tunnelling recombination sites

The anomalous fading (AF) of thermoluminescence (TL) and optically stimulated luminescence (OSL) signals in Durango apatite is attributed to tunnelling effects. Electrons from the TL and OSL traps in this material are transferred, via a tunnelling effect, to the recombination sites. The availability of recombination sites for tunnelled electrons is of major importance for the degree of AF rate observed in this material. It is expected that a variation of the number of the electron recombination sites will be reflected in the experimentally measured AF rate. In the present work an investigation of the recombination sites for the tunnelled electrons is attempted by studying the AF effect using a special technique, in which the anomalously faded TL (OSL) is replaced by an equal amount of TL (OSL) induced by a beta dose.     

Thermoactivated spectroscopy of heterovalent impurity traps in CdWO4

Abstract

Recombination luminescence emission spectra, TSL and trap spectra estimated by fractional glow technique (FGT), in nominally pure and Li-, Bi- and Ho-doped CdWO₄, crystals are reported. According to the investigations by FGT heterovalent impurities Li, Bi and Ho causes localized electronic states which act as traps for charge carriers. It is shown that TSL results in emission of known blue-green luminescence band by emptying of the Li⁺-related traps in CdWO₄-Li and yellow luminescence band by emptying of the Bi³⁺-related traps in CdWO₄-Bi. It is proposed that blue-green and yellow luminescence occur by recombination correspondingly of free holes and free electrons at different intrinsic tungstate group related luminescence centers.     

Modelling the thermal bleaching of OSL signal in the case of a competition between recombination centres

The thermal bleaching of the optically stimulated luminescence (OSL) has been investigated by computer simulations for a model including three traps and two luminescence centres. The deepest trap is active only during the OSL process. Two other traps are active only during the thermal bleaching. The thermal bleaching effects on the OSL intensity as well as on the OSL curve shape are presented for the wide range of trap and luminescence centre parameters and for the different settings of optical detection window. The conventional OSL curve analysis consisting in decomposition of the OSL curve into first order components is applied to the simulation results and the optical cross section spectra obtained as a result of this analysis are compared with the model assumptions. The simulations show that OSL signal can decrease to undetectable level even when the traps related to this signal are not emptied during thermal bleaching. The residual level of the OSL signal after bleaching process, however, depends strongly on centre parameters and concentrations. The modifications of optical detection spectral window lead to significant changes of bleaching effects. The thermal bleaching influences also the optical cross section spectra obtained as a result of the OSL curve decomposition.     

Features of OSL and TL properties of anion-defective corundum crystals exposed to thermo-optical treatment

The results of systematic investigation of the mechanisms and role of phototransfer in TL and OSL processes in α-Al₂O_3−δ crystals under controlled filling of the main and deep traps depleted at 450 and 720 K, respectively, are presented.Optical depletion spectra of the main and deep traps were measured and compared. It was found that green light stimulation only depletes the main trap, while blue light depletes both the main and deep traps. Optical depletion of the deep trap results in phototransfer of charges that can be realized by 2 mechanisms: either through the main trap to recombination centers or directly to the latter. However, the dominant contribution to the OSL signal is provided by phototransfer through the main trap. It is also found that UV emission at 3.7 eV dominates over F-emission at 3.0 eV in the phototransferred TL spectrum. It is assumed that this UV emission is not related to the F⁺ centers.     

Dose-rate effect in the model of semi-localized transitions (SLT)

The model of semi-localized transitions (SLT) unifies two standard models of thermoluminescence (TL) and optically stimulated luminescence (OSL) kinetics – the simple trap model (STM) and the model of localized transitions (LT). SLT equations were previously formulated for the heating stage of TL. This paper presents SLT equations for the excitation and fast relaxation stages. Exemplary calculations were performed to show the occurrence of dose-rate effect – previously found in STM. It is shown that the dose-rate effect occurs for both – localized and delocalized TL glow peaks.     

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.     

Luminescence properties of common glasses for application to retrospective dosimetry

Seventeen domestic and scientific glass specimens were investigated for thermoluminescence (TL) properties suitable for application to retrospective population dosimetry. Usefulness for retrospective dosimetry was initially judged by the presence of well-defined TL glow peaks and the absence of irradiation-independent luminescence. Of particular interest were TL glow peaks having relatively low trap depths, to prevent significant natural dose accumulation. Minimum useful trap lifetimes would be in the order of weeks. Surveys were undertaken to observe the TL and optically stimulated luminescence (OSL) behaviour of each sample. Most samples showed identifiable TL, with Pyrex in particular, and samples from a jar, a lampshade, and opaque blue beads all showing well-defined TL glow peaks with sensitivities that were not significantly affected by prior irradiation and heating of the sample. Kinetic analysis of these samples showed that their TL emission originates from traps with suitable stability for retrospective dosimetry. It is concluded that, while some glass samples show promising results, the inherent variability of an amorphous substance such as glass means that the suitability of each sample must be determined on a case-by-case basis.     

Comparison of the properties of various optically stimulated luminescence signals from potassium feldspar

Various optically stimulated luminescence signals from K-feldspar have been used to determine the equivalent doses of sediment samples. Understanding the properties of these optical signals is critical to evaluate their applicability and limitations to optical dating. In this paper, some properties of IRSL, post-IR OSL and post-IR IRSL signals (detected in the UV region using U-340 filters) from a museum sample of K-feldspar were investigated by analyzing the relationships between optical and TL signals, and the effect of optical bleaching and heating on optical signals. The trap parameters of the different optical signals were calculated using the pulse annealing method. The results show that this sample exhibits two regenerated TL peaks at ～140 and ～330 °C. Corresponding to the low temperature TL peak, the OSL and post-IR OSL signals appear to be more associated with lower temperature TL than the IRSL signal measured at 50 °C. Corresponding to the high temperature TL peak, the post-IR IRSL signals mainly originate from the more thermally stable traps associated with the high temperature TL, compared with the IRSL and post-IR OSL signals. However, the post-IR IRSL_225 °C signal is shown to be hard to be bleached by blue light and simulated sunlight, compared with the IRSL_50 °C and low temperature post-IR IRSL signals. The implication for optical dating is that the elevated temperature post-IR IRSL signals can be preferentially applied over other signals from K-feldspar, but it is desirable that the effectiveness of the pre-depositional zeroing of these signals is assessed.     

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.     

Optically stimulated luminescence (OSL) study of synthetic stishovite

Optically stimulated luminescence (OSL) of synthetic stishovite was investigated for a future dating technique of meteor impact craters. Luminescence around 330 nm was measured on the γ-ray irradiated stishovite under two stimulating light sources of infrared laser (830 nm) and blue light emitting diode set (470 nm). Thermoluminescence (TL) studies before and after the OSL measurements showed the intensities around 100–200°C and 220–350°C to increase and those around 350–450°C to decrease. This indicates that a part of deep-trapped charges excited during the OSL measurements were retrapped by shallower traps. The infrared stimulated luminescence (IRSL) after the TL measurement up to 450°C could not be detected, while the blue light stimulated luminescence (BLSL) after TL had about one-tenth of the intensity before TL. This indicates that a part of the charges in shallower traps were detrapped thermally and returned to the deeper traps which were related to BLSL. The result implies that some of the BLSL-related traps are quite stable at room temperature and could be used for geological dating. In addition, two paramagnetic centers produced by sudden release of high pressure in synthesis process were found in the unirradiated stishovite by electron spin resonance (ESR). Their g-factors are g=2.00181 and g=2.00062 for an axial signal and g=2.00305 for the other isotropic signal. These signals could be used for an evidence of impacts if those signals could be stored in geological time.     

LiMgPO_4:Tm,Tb的热释光和光释光陷阱参数

采用高温固相法合成了LiMgPO_4:Tm,Tb粉末样品,测定了热释光陷阱参数激发能E和频率因子s.用脉冲退火和多次退火方法研究了其光释光陷阱参数E和s,并与用多速法得到的热释光的结果进行了比较.对不同β射线剂量照射的样品发光曲线的研究表明,300°C高温峰属于一级动力学发光峰.通过对热释光和光释光陷阱的相关性研究表明,经200°C预热的热释光信号(对应于300°C高温峰)和光释光信号很有可能来自于同一深度的陷阱.     

The influence of electron–phonon interaction on the OSL decay curve shape

The significance of the electron–phonon interaction for optically stimulated luminescence (OSL) process in quartz is demonstrated. OSL variation with temperature has been investigated for four samples of natural quartz. Changes of the OSL decay rate have been observed for all components of the OSL signal. The scale and tendency of these changes are comparable with outcomes of computer simulations carried out for the model composed of two deep electron traps, one shallow trap and one recombination centre, taking into account the electron–phonon interactions.     

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.     

TL/OSL properties of crystalline inclusions from heavy,barytes loaded,concrete

In the present work, we report the luminescence data obtained from heavy, barytes loaded, concrete containing many crystalline inclusions, extracted from a shielding block located at CERN. The use of both Thermoluminescence (TL) and Optically Stimulated Luminescence (OSL) signals, resulting from a specific trap at about 200 °C, is investigated for retrospective dosimetry purposes. By applying thermal cleaning experiments the TL signal of interest was isolated. Basic TL and OSL properties as thermal and optical stability, repeatability and mainly the linearity of the TL and OSL signals as a function of beta dose were investigated. The implications of all these luminescence properties to retrospective dosimetry are also briefly discussed.     

On the validity of the general order kinetics for analyzing phosphorescence curves

The parameters characterizing trap and recombination centers, such as activation energies, recombination and trap probabilities, involved in thermoluminescent materials can be found by analyzing phosphorescence curves with an adopted model consisting of trap and recombination centers, and assuming the mechanisms involved in the carrier traffic (kinetics). Nowadays the most employed kinetics is the General Order kinetics (GO). Since this model is heuristic, this article reports how successful it is in providing reliable values for the traps parameters. The equations describing the traffic of carriers were used to generate simulated phosphorescence curves for specific values of trap and recombination parameters. These simulated phosphorescence curves were later analyzed with the GO kinetics, and the resulting parameters compared to the correct ones in order to evaluate the validity of the model.     

Modelling the optical bleaching of the thermoluminescence of K2YF5:Pr3+

Optical bleaching of the thermoluminescence (TL) curve of K₂YF₅:Pr³⁺ has been observed after optically stimulated luminescence (OSL) readout of pre-irradiated crystals. The traps being responsible for the TL signal are not emptied completely by the optical stimulation. Furthermore, if the illumination time is increased a constant intensity level of the residual TL glow curve is eventually achieved. On the other hand, if the low temperature peak of the glow curve is thermally cleaned, no subsequent OSL is measured. This behavior has been successfully explained by assuming that part of the electrons in the trap being responsible for the low temperature glow peak of K₂YF₅:Pr³⁺ recombine with holes via localized transitions during optical stimulation. During TL all trapped electrons recombine via delocalized transitions. Simulations have been carried out in order to demonstrate the feasibility of the model.