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).     

Post-irradiation storage and thermal stability of thermoluminescence glow peaks in LiF:Mg,Cu,Si

Newly developed LiF:Mg,Cu,Si was found to exhibit no significant fading on room temperature post-irradiation storage up to several months. In view of the wide variation in the reported data of fading of LiF:Mg,Cu,P exhibiting glow curve structure similar to that of LiF:Mg,Cu,Si, a study of the effect of post-irradiation storage and thermal treatments on the deconvoluted glow peaks of LiF:Mg,Cu,Si was undertaken. The decay of inseparable peak-3 by post-irradiation storage or thermal treatments did not indicate any rearrangement in the trap occupation that would affect the response of the main peak (peak-4). A post-irradiation treatment at 125 °C for 10 min was found to be the optimum to eliminate the lower temperature peaks.     

The dependence of thermoluminescence of LiF:Mg,Cu,Si on sintering temperatures and dopants concentrations

The dependence of thermoluminescence (TL) of LiF:Mg,Cu,Si on sintering temperatures and dopants concentrations were investigated. The dependency of the TL in LiF:Mg,Cu,Si on sintering temperature exhibits a very sharp maximum at 830 °C. LiF:Mg,Cu,Si is much too sensitive than LiF:Mg,Cu,P to sintering temperature. The glow curve and the TL sensitivity depend on the concentration of Mg, Cu and Si, showing a distinct maximum for certain concentrations of these impurities. Mg seems to be the most essential dopant, as very small changes of the Mg content strongly influence both the glow curve and the TL sensitivity. Si is the main activator responsible for TL emission. The stability to heat treatments in LiF:Mg,Cu,Si was influenced greatly by Mg concentrations. The thermal instability in LiF:Mg,Cu,Si is caused not by Cu and Si but Mg ion state change. It was found that the optimum concentrations are Mg:0.6 mol%, Cu:0.03 mol% and Si:0.9 mol% for this material, which showed the best stability to heat treatment.     

Newly developed highly sensitive LiF:Mg,Cu,Si TL discs with good stability to heat treatment

The preparation method and some dosimetric properties of the new LiF:Mg,Cu,Si discs are presented. The effect of heat treatments on LiF:Mg,Cu,Si was investigated. The shape of the glow curve for LiF:Mg,Cu,Si is similar to that for standard LiF:Mg,Cu,P (GR-200A), and shows minimal differences when annealed in the range from 260 °C to 290 °C for 10 min. The TL sensitivity for LiF:Mg,Cu,Si is much lower than that for GR-200A, but is 35 times larger than that for TLD-100 and is slightly higher than that for HMCP. The height of the high-temperature peaks for LiF:Mg,Cu,Si is not only lower than that for GR-200A, but also lower than that for HMCP. The glow curve shape of LiF:Mg,Cu,Si annealed at 260 °C for different times shows minimal differences and TL response remains stable. These results indicate that the new LiF:Mg,Cu,Si disc has a good stability to thermal treatments and a lower residual TL signal.     

Optimization of preparation procedure of LiF:Mg,Cu,Si TLD for improving the reusability

Several thermal treatments in the temperature range from 270 °C to 320 °C (each of 10 min) were tested as a final preparation procedure of LiF:Mg,Cu,Si to improve the protocol of TL readout with less residual signal for the LiF:Mg,Cu,Si TLD. This high sensitivity LiF:Mg,Cu,Si TLD exhibited thermal stability much better than that of the well known LiF:Mg,Cu,P. For LiF:Mg,Cu,Si, a readout temperature up to 300 °C did not affect the TL sensitivity and glow curve structure for 12 cycles of exposure and readout following an initial thermal treatment at 295 °C for 10 min. The residual TL signal also remained negligible.     

Investigations of thermoluminescence properties of multicrystalline LiF: Mg,Cu, Si phosphor prepared by edge defined film fed growth technique

Thermoluminescence (TL) properties of LiF: Mg, Cu, Si phosphor prepared in multicrystalline form using edge defined film fed growth (EFG) technique has been investigated. The effect of preparation route on TL properties and thermal stability has been studied. To improve the TL dosimetry properties, phosphor is subjected to different annealing temperatures ranging from 250 °C to 450 °C. The shape of the glow curve structure and peak temperature remains similar at different annealing temperatures, however peak intensities vary. The consistency in the glow curve structure with annealing temperature elucidate that TL trapping states are stable in nature. Thermal annealing at 300 °C for 10 min gives maximum TL intensity with main dosimetry peak at 209 °C. The TL intensity of the main dosimetry peak is increased by a factor of five as compared to as-grown crystal. The thermal stability of LiF: Mg, Cu, Si is found to be better than LiF: Mg, Cu, P. Trapping parameters are calculated to have an insight study of defect states. A simple glow curve structure, tissue equivalency, thermal stability, low residual signal, linear response and reusability makes LiF: Mg, Cu, Si a suitable phosphor for radiation therapy, radio diagnostics and personnel dosimetry applications.     

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.     

The glow curve structure for the LiF:Mg,Cu,Na,Si TL detector with dopants concentrations and sintering temperatures

The glow curve structures for LiF:Mg,Cu,Na,Si TL detectors with various dopant concentrations and sintering temperatures were investigated for the improvement of the glow curve structure and sensitivity of the TL detector. The dopant concentrations were varied over the following ranges: Mg (0–0.25 mol%), Cu (0–0.07 mol%), Na and Si (0–1.5 mol%). With increasing Cu concentration, the intensity of the main peak was intensified and reached a maximum at a concentration of 0.05 mol%. The high-temperature peak was reduced. The dependency of the main peak intensity on the Mg concentration exhibits a sharp maximum at 0.2 mol%. The intensity of the high-temperature peak tends to rise slightly with increasing Mg concentration. It was found that the optimum concentrations of the dopants in the LiF:Mg,Cu,Na,Si TL material are Mg: 0.2 mol%, Cu: 0.05 mol%, Na and Si: 0.9 mol%. The dependency of the main peak intensity on sintering temperature exhibits a very sharp maximum at 830°C. The high-temperature peak was rapidly reduced after 825°C.     

A new method for the numerical analysis of thermoluminescence glow curve

A new method to analyze the thermoluminescence (TL) glow curve has been presented. It has been shown that this method is efficient and fast in generating the TL glow curves and can be adopted in a numerical curve fitting for obtaining the relevant TL parameters of a given TL glow curve data. This new method is based on a general approximation (GA) which assumes only that the concentration of the electrons in the conduction band is negligible when compared with the concentration of the electrons in the traps. The GA method has been tested against the reference glow curve data which was generated by the full iteration method without any prior approximation in the one-trap-one-recombination-centre model. By finding the best fit between the reference data and the curves generated by the GA method, the values of the kinetics parameters have been determined. Also, the general order kinetics (GOK) and the peak shape method have been examined. The fitted values of the activation energy and the initial concentration of electron by the GA method match reasonably well with the original value.     

OSL signal of lithium fluoride and its relationship with TL glow-curves

The widely known LiF TL detectors: LiF:Mg,Ti (MTS-N) and LiF:Mg,Cu,P (MCP-N), were investigated with respect to their OSL properties. It was found that both materials exhibit quite substantial OSL sensitivity. In particular, in the case of LiF:Mg,Cu,P this sensitivity was very high, significantly exceeding that of BeO, the standard OSL dosimetric material. LiF:Mg,Cu,P could be a very promising candidate for application in dosimetry, if not for the fading, which was found to be quite high, reaching nearly 80% loss of the signal within 60 h. The OSL signal intensity shows a correlation with the peak 2 of the TL glow curves indicating that the same trapping sites are responsible for both processes. Peak 2 of LiF:Mg,Ti shows a peculiar property, that blue light stimulation removes only about half of its initial intensity, disregarding the duration of stimulation. This suggests, that this peak may have a composite structure and originates from both light-sensitive and light-insensitive trapping centres.     

Energy levels in YPO4:Ce3+,Sm3+ studied by thermally and optically stimulated luminescence

Energy-resolved optically stimulated luminescence (OSL) spectra and thermoluminescence (TL) glow curves of a powder sample of YPO₄:Ce³⁺,Sm³⁺ were measured to investigate the nature of the trapping centre and to locate its energy level relative to the valence and conduction bands of the YPO₄ host. The high-temperature glow peak could unequivocally be assigned to Sm²⁺ (thus Sm³⁺ acts as an electron trap). The trap depth of this centre, as derived from the OSL excitation spectra, is in good agreement with the Dorenbos model prediction. The OSL excitation spectra also reveal excited states of Sm²⁺ well below the conduction band. These excited states produce a broadening of the high-temperature TL glow peak and also cause the activation energy determined by the Hoogenstraten method to underestimate the trap depth.     

Thermoluminescence Kinetic Parameters of TLD-600 and TLD-700 after ~(252)Cf Neutron+Gamma and ~(90)Sr-~(90)Y Beta Radiations

The thermoluminescent(TL) properties such as glow curve structure, relative thermoluminescence sensitivity,dose response linearity of lithium fluoride thermoluminescent dosimeters 6 LiF:Ti,Mg(TLD-600) and 7 LiF:Ti,Mg(TLD-700) are investigated after irradiation ~(252)Cf neutron+gamma and ~(90)Sr-~(90)Y beta sources at room temperature and then the obtained results are compared. The kinetic parameters, namely the order of kinetics b,activation energy Ea and the frequency factor s,are calculated using the computerized glow curve deconvolution(CGCD) program. The effect of heating rate on the glow curves of dosimeters is also investigated. The maximum TL peak intensities and the total area under the glow curves decrease with the increasing heating rate. There is no agreement with the kinetic parameters calculated by the CGCD program for both radiation sources.     

Effect of dopants on TL characteristics of LiF:Mg,Cu,P detectors

LiF:Mg,Cu,P detectors produced at the Institute of Nuclear Physics in Krakow have shown very good dosimetric characteristics. Understanding of the effect of the concentration and type of dopants is important in the characterization of TL materials. The aim of work was to investigate the influence of the type and concentration of the dopants on the photon energy response of these detectors by irradiations “in air” and on the ISO water phantom in the range of mean photon energies between 33 and 164 keV. The influence of dopants on the glow curves, sensitivity and reproducibility was also examined. Results showed that measured energy dependence values are lower compared to the theoretical values both “in air” and on phantom. The type and concentration of the dopants influence the shape of the glow curves and sensitivity while for energy dependence is more important the presence of certain activators, namely copper.     

Investigation of thermoluminescence in Li_2B_4O_7 phosphors doped with Cu, Ag and Mg

Li_2B_4O_7 (LBO):Cu,Ag,Mg phosphors have been prepared by the sintering technique. The roles of the Ag and Mg dopants in the phosphors have been studied using the methods of thermoluminescence (TL) glow curves and TL 3D spectra. The results indicated that proper concentrations of Ag and Mg can enhance the TL of LBO:Cu. It was also indicated that the intensity of TL peak at ~130℃ is reduced with the in- creasing Ag concentration, and enhanced with the increasing Mg concentration. From the TL 3D spectra, three emission bands (λ1 = 421 nm, λ2 = 380 nm, λ3 = 350 nm) were observed: the intensity of low energy emission band is reduced and that of the high energy is enhanced with the increasing dopant Ag; on the contrary, the intensity of low energy emission band is enhanced and that of the high energy one is reduced with the increasing dopant Mg.     

Dose response of thermoluminescence emission spectra of LiF:Mg,Ti with different Mg, Ti impurity concentrations

The dose response of the TL emission spectra of an LiF:Mg,Ti (TLD-100) sample and three LiF:Mg,Ti samples with different impurity concentrations (0–6 ppm Ti and 80–100 ppm Mg) have been measured. At a dose less than 22 Gy the emission spectrum of the TLD-100 sample comprises one emission band at 420 nm. The sample without Ti shows also one emission band but now at 620 nm. The spectra of the other two samples comprises two emission bands at 420 nm and 620 nm of which the intensity of the 420 nm band increases with increasing Ti concentration. The dose response of the glow peaks is different for peaks at different temperatures and emission bands. From these observations it can be concluded than in LiF:Mg,Ti at least some of the traps and luminescent centers are coupled.     

Cu+ emission in Li2BPO5 material for thermoluminescence dosimetry

In this study, Li₂BPO₅ doped with Cu and that co-doped with Mg are synthesized by the wet chemical technique and exposed to γ rays of ⁶⁰Co to determine their thermoluminescence (TL) properties. The X-ray diffraction technique shows the crystalline nature of the prepared material. The photoluminescence (PL) emission spectra of Li₂BPO₅:Cu phosphor show the strong prominent peak at 368 nm in the violet region of the visible spectrum due to the transition of 3d⁹4s¹ ? 3d¹⁰ of monovalent copper ion. The PL emission of Li₂BPO₅:Cu is enhanced by the addition of Mg. The TL glow curves of γ-irradiated Li₂BPO₅:Cu sample show one glow peak at 143°C, indicating that only one set of traps is being activated within the particular temperature range each with its own value of activation energy (E) and frequency factor (s). The trapping parameters associated with the prominent glow peak of Li₂BPO₅:Cu are calculated using the glow curve shape (Chen's) method. The release of hole/electron from defect centers at the characteristic trap site initiates the luminescence process in these materials. A linear TL response is observed in Li₂BPO₅:Cu in a long span of exposures. The sensitivity of Li₂BPO₅:Cu sample is observed to be 7.8 times that of (TLD-100) LiF:Mg, Ti.     

Study of a new Lif:Mg,Cu,P formulation with enhanced thermal stability and a lower residual TL signal

This paper presents results obtained for a new LiF:Mg,Cu,P (HMCP) preparation with modified Mg and Cu concentrations. The shape of the HMCP glow curve shows minimal differences for annealing in the range from 523 to 543 K for 10 min. The thermoluminescence (TL) readout value remained stable when annealed in the range from 513 to 543 K for 10 min. The new formula allows heating of the material to higher temperatures than that originally employed for the well-known GR-200A dosemeter, practically without losses in sensitivity. The TL sensitivity is approximately half of that for the GR-200A, and still 29-fold greater than that for the TLD-100 dosemeter, and the residual signal is approximately five-fold lower than for the GR-200A. These results indicate that the new TL material shows enhanced thermal stability and a lower residual TL signal at a small TL sensitivity cost. The heat treatment temperatures are related to concentrations of Mg and Cu in LiF:Mg,Cu,P.     

An improved experimental procedure of separating a composite thermoluminescence glow curve into its components

We present an improved experimental procedure of separating a composite thermoluminescence glow curve into its components. Careful monitoring of the isothermal cleaning process using the initial rise method ensures the complete thermal removal of TL peaks. Digital subtraction of two experimental TL glow curves yields individual experimental TL glow peaks. Several standard methods (initial rise and whole glow curve) are used to obtain the energy values and frequency factors of the traps. The method has been used successfully to analyze the well-known composite TL glow curve of the dosimetric material LiF (TLD-100). The limitations of the method are illustrated by analyzing the highly complex TL glow curve of a UV irradiated synthetic calcite consisting of at least 6 TL peaks. Although the method works best for TL glow curves described by first order kinetics, it should also be applicable to more general kinetics.     

Development of a personal dosimeter badge system using sintered LiF:Mg,Cu,Na,Si TL detectors for photon fields

The badge system of personal thermoluminescence (TL) dosimeter for photon fields using LiF:Mg,Cu,Na,Si TL material, which was developed by Korea Atomic Energy Research Institute (KAERI) a few years ago, was developed by taking advantage of its dosimetric properties including energy dependencies. A badge filter system was designed by practical irradiation experiments supported by computational modeling using Monte Carlo simulation. Design properties and dosimetric characteristics such as photon energy response and angular dependence of new TL dosimeter system examined through the irradiation experiments are presented. Based on the experiments for the developed dosimeter, it is demonstrated that the deep dose response of dosimeter provided the value between 0.78 and 1.08, which is within the design limit by ISO standard. This multi-element TL dosimeter badge system allows the discrimination of the incident radiation type between photon and beta by using the ratios of the four TL detectors. Personal TL dosimeter using sintered LiF:Mg,Cu,Na,Si TL detectors has the ability to measure a personal dose equivalent H_p(d) for a wide range of photon energies.     

Si–Si bond as a deep trap for electrons and holes in silicon nitride

A two-stage model of the capture of electrons and holes in traps in amorphous silicon nitride Si₃N₄ has been proposed. The electronic structure of a “Si–Si bond” intrinsic defect in Si₃N₄ has been calculated in the tight-binding approximation without fitting parameters. The properties of the Si–Si bond such as a giant cross section for capture of electrons and holes and a giant lifetime of trapped carriers have been explained. It has been shown that the Si–Si bond in the neutral state gives shallow levels near the bottom of the conduction band and the top of the valence band, which have a large cross section for capture. The capture of an electron or a hole on this bond is accompanied by the shift of shallow levels by 1.4–1.5 eV to the band gap owing to the polaron effect and a change in the localization region of valence electrons of atoms of the Si–Si bond. The calculations have been proposed with a new method for parameterizing the matrix elements of the tightbinding Hamiltonian taking into account a change in the localization region of valence electrons of an isolated atom incorporated into a solid.