Monte Carlo simulations of TL and OSL in nanodosimetric materials and feldspars

The study of luminescent materials consisting of nanoclusters is an increasingly active research area. It has been shown that the physical properties of such nanodosimetric materials can be very different from those of similar conventional microcrystalline phosphors. In addition, it has been suggested that traditional energy band models may not be applicable for some of these nanodosimetric materials, because of the existence of strong spatial correlations between traps and recombination centers. The properties of such spatially correlated materials have been previously simulated by using Monte Carlo techniques and by considering the allowed transitions of charge carriers between the conduction band, electron traps and recombination centers. This previous research 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. This paper presents a simplified method of carrying out Monte Carlo simulations for thermoluminescence (TL) and optically stimulated luminescence (OSL) phenomena, based on a recently published model for feldspar. This model is based on tunneling recombination processes involving localized near-neighbor transitions. The simulations show that the presence of small clusters consisting of a few traps can lead to multiple peaks in both the TL and linearly modulated OSL signals. The effects of donor charge density, initial trap filling and cluster size are simulated for such multi-peak luminescence signals, and insight is obtained into the mechanism producing these peaks.     

On luminescence stimulated from deep traps using thermally-assisted time-resolved optical stimulation in α-Al2O3:C

We report a study of charge transfer mechanisms of electrons stimulated optically from very deep traps, also known as donor traps, in α-Al₂O₃:C. The investigations were carried out using thermally-assisted time-resolved optical stimulation, thermoluminescence and by way of residual thermoluminescence from the main electron trap. When the charges are optically stimulated from the deep traps, they are redistributed via the conduction band to the main electron trap and the shallow trap from where they are optically or thermally released for recombination at luminescence centres. The luminescence is strongly quenched at high measurement temperature as evident by very short luminescence lifetimes at these temperatures. The main peak due to residual thermoluminescence is located at a higher temperature than the conventional main peak.     

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).     

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.     

Optical depth of traps in AL2O3:C determined by the variable energy of stimulation OSL (VES-OSL) method

Standard methods of OSL measurements (CW-OSL or LM-OSL) do not allow for the direct determination of optical depth of traps. The variable energy of stimulation optically stimulated luminescence (VES-OSL) method gives such possibility. It consists in optical stimulation with the continuous increase of stimulation light energy and is analogous to the glow curve method in TL measurements. The VES-OSL curve shape and maximum position can be regulated by the stimulation photon flux, the rate of stimulation energy increase and by measurement temperature. This allows for detecting the OSL from very deep traps that give the TL signal overlapping with strong incandescence. The VES-OSL measurements carried out for Al₂O₃:C showed that traps having the optical depth between 2.0 and 2.8 eV are responsible for the OSL signal related to TL peak at about 200 °C. The OSL signal from the much deeper traps from the range 2.8–3.3 eV was also detected. The TL signal related do these traps cannot be detected below 500 °C.     

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.     

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.     

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.     

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.     

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.     

Non-linear light modulation OSL phenomenon

A theoretical simulation and experimental verification of non-linear light modulation of optically stimulated luminescence (NL-OSL) technique has been demonstrated under first- and general-order kinetics. It is found that the NL-OSL technique gives all the information that can be obtained from the conventional LM-OSL technique with some useful features and flexibilities. It is observed that the NL-OSL curve is more symmetric than the LM-OSL curve. The NL-OSL technique can be useful in analyzing OSL traps having very low and closely lying values of photo-ionization cross-sections of meta-stable traps obeying different order of kinetics.     

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.     

A new look at the linear-modulated optically stimulated luminescence (LM-OSL) as a tool for dating and dosimetry

Optically stimulated luminescence (OSL) has been in use for dosimetry and dating in the last two decades. Since the OSL dependence on time is a featureless decaying function, a linear-modulation of the stimulating-light intensity has been suggested [Bulur, E., 1996. An alternative technique for optically stimulated luminescence. Radiat. Meas. 26, 701–709.], which resulted in a peak-shaped curve. The properties of this curve have been studied, assuming first-, second- and general-order kinetics. In a recent paper we have shown [Chen, R., Pagonis, V., 2008. A unified presentation of thermoluminescence (TL), phosphorescence and linear-modulated OSL (LM-OSL). J. Phys. D: Appl. Phys. 41, 035102 (1–6).] that for general-order curves, the peak maximum cannot be expected to depend linearly on the dose of excitation. A new presentation of the LM-OSL has been suggested, in which the peak maximum is linear with the filling of trapping states, which, in turn, may be expected to be linear with the dose under appropriate conditions. In the present work, we report on results of numerical simulation of the LM-OSL using the one trap-one recombination center (OTOR) model, dealing with the traffic of carriers between one trapping state, one kind of recombination center and the conduction and valence bands during excitation and read-out, and without making any simplifying assumptions. The process during optical read-out has been followed in the simulation that consisted of the numerical solution of the relevant sets of coupled differential equations, and also by analytical treatment. Sets of parameters leading to approximately first- and second-order kinetics, and to intermediate cases, have been used and the results presented in the original and the new ways are shown. The consequences concerning dating and dosimetry are discussed.     

A computer program for the deconvolution of the thermoluminescence glow curves by employing the interactive trap model

An efficient computer program has been developed to deconvolute thermoluminescence (TL) glow peaks and optically stimulated (OSL) curves by employing a method of the interactive trap model (ITM). The program is designed to be used easily on the MS Windows-based computer with a graphical user interface. This program could be used to analyze the TL glow curves by using the traditional first-order kinetics (1OK), second-order kinetics (2OK), general order kinetics (GOK), mixed order kinetics (MOK) and the general approximation (GA) method as well as ITM. The program was tested with the generated data and the experimental results of deconvoluted TL glow curves of LiF TLD-100 by assigning five interacting traps and one recombination center. A complete version with full functionalities of this program can be downloaded from the web site http://physica.gnu.ac.kr/TLanal.     

Nonlinear dose dependence of TL and LM-OSL within the one trap-one center model

In a recent paper, it has been shown that strong sub-linearity of the occupancy n₀ of trapping states far from saturation can be explained by the simplest model of one trap-one recombination center (OTOR). In the present work we report on results of numerical simulation of dose dependence of the TL maximum under similar conditions. In some cases, the TL maximum is found to be strictly proportional to the filling of the traps, but this is not always the case. Different sublinear dose-dependence functions of the trap occupancy and the maximum TL are demonstrated. With the same sets of parameters, curves of LM-OSL have also been simulated; superlinear as well as sublinear dependencies on the excitation dose have been found.     

The effects of deep trap population on the thermoluminescence of Al2O3:C

The influence of deep traps on the 450 K thermoluminescence (TL) peak of Al₂O₃:C is studied. Depending upon the sample and on the degree of deep trap filling, features such as the TL width, area and height can vary considerably. These effects are interpreted to be due to: (a) sensitivity changes introduced by competition mechanisms involving deep electron and hole traps, and (b) the multiple component nature of the 450 K TL peak. The influence of the deep traps on the TL was studied using different excitation sources (beta irradiation or UV illumination), and step annealing procedures. Optical absorption measurements were used to monitor the concentration of F- and F⁺-centers. The data lead to the suggestion that the competing deep traps which become unstable at 800–875 K are hole traps, and that the competing deep traps which become unstable at 1100–1200 K are electron traps. Both the dose response of the TL signal and the TL sensitivity are shown to be influenced by sensitization and desensitization processes caused by the filling of deep electron and hole traps, respectively. Changes in the TL peak at low doses were also shown to be connected to the degree of filling of deep traps, emphasizing the influence of deep trap concentration and dose history of each sample in determining the TL properties of the material. Implications of these results for the optically stimulated luminescence properties are also discussed.     

Complex OSL signal and a trap independence assumption

Simulations of optically stimulated luminescence process were performed for the model which includes two electron traps and one recombination centre. The fulfillment of the trap independence assumption was tested. The fitting procedure was applied for the simulation outputs in order to check if they can be decomposed into the first-order components. A wide range of trap parameters was applied and it was shown that the trap independence assumption is valid only for some special cases but the simulated OSL curves fit often with high accuracy a sum of first-order components which differ significantly from these used in the model.     

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.