Influence of sintering temperatures on LiF:Mg,Cu,P with various magnesium concentrations

The dependence of LiF:Mg,Cu,P samples with various concentrations of Mg on sintering temperatures was investigated to find a new dosimeter. The influence of high sintering temperatures on LiF:Mg,Cu,P chips depends strongly on Mg concentrations. The height of the main peak versus the sintering temperatures exhibits a maximum, the position of which varies between 690 °C and 750 °C, depending on the Mg concentration in the range studied. The high temperature peaks of LiF:Mg,Cu,P for various Mg concentrations reduce basically when the sintering temperature is increased. LiF:Mg,Cu,P is much less sensitive than LiF:Mg,Cu,Si to sintering temperature. LiF:Mg,Cu,P with 0.6 mol% of Mg can be re-used at annealing temperature of 260 °C, regardless of the sintering temperature. It was found that the optimum concentration is Mg: 0.6 mol%, the optimum sintering temperature is 750 °C, considering that LiF:Mg,Cu,P with a low residual signal and good sensitivity can be re-used at annealing temperature of 260 °C and produced in a large scale. The new optimum LiF:Mg,Cu,P formation has 52 times higher than that of the TLD-100, and an extremely low residual signal of 0.07% without an initialization readout procedure.     

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.     

Dosimetric properties of the newly developed KLT-300 (LiF:Mg,Cu,Na,Si) TL detector

The dosimetric properties of the newly developed KLT-300 (KAERI LiF:Mg,Cu,Na,Si TL detector) in KAERI (Korea Atomic Energy Research Institute) were investigated. The sensitivity of the TL detector was about 30 times higher than that of the TLD-100 by light integration. In the study of the dose linearity of the detector, the dose response was very linear up to 10 Gy and a sublinear response was observed at higher doses. The energy response of the detector was studied for photon energies from 20 to 662 keV. The results show that a maximum response of 1.004 at 53 keV and a minimum response of 0.825 at 20 keV were observed. The reproducibility study for the TL detector was also carried out. The coefficients of variation for each detector separately did not exceed 0.016, and for all the 10 detectors collectively it was 0.0054. IEC Standard requires that the coefficient of variation shall not exceed 0.075. So, the reproducibility of this new TL detector sufficiently satisfied the IEC requirements. A detection threshold of the detector was investigated and found to be 70 nGy by Harshaw 4500 TLD Reader.     

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.     

Thermoluminescence glow curve deconvolution of LiF:Mg,Cu,Si with more realistic kinetic models

Thermoluminescence (TL) glow curves of LiF:Mg,Cu,Si were deconvoluted with the introduction of enhanced physical model which envisages that both electrons and holes, produced by ionization radiation and trapped at the respective traps, can be thermally released into the conduction and the valence band, respectively and the holes may also radiatively recombine with electrons at the electron recombination centers. The model is more generalized than the ordinary trap interaction model which only permits the traffic of electrons through the conduction band. An effective numerical analysis method was developed to calculate the glow curve to be compatible with the measured curves. The validity of the numerical method was verified through artificially generated TL glow curves for a wide range of trap parameters. In order to identify TL kinetics of LiF:Mg,Cu,Si with higher accuracy, its glow curves were deconvoluted for two more generalized models, namely, the Schön–Klasens model and the Chen–Pagonis–Lawless model as well as the ordinary trap interactive model. The parameters in the more generalized multi-trap multi-recombination center (MTMR) model were found to be consistent with the quasi-static approximation(QSA) method.     

Dependence of the thermoluminescent high-temperature ratio (HTR) of LiF:Mg,Ti detectors on proton energy and dose

The high-temperature ratio (HTR) is a parameter quantifying changes of the shape of the high-temperature part of the LiF:Mg,Ti glow-curve after exposure to densely ionizing radiation. It was introduced in order to estimate the ‘effective LET’ of an unknown radiation field and to correct the decreased relative TL efficiency for high-Linear Energy Transfer (LET) radiation.In the present work the dependence of HTR on proton energy (14.5–58 MeV) and dose (0.5–30 Gy) was investigated. All measured HTR values were at the level of 1.2 or higher, therefore significantly different from the respective value for gamma-rays (HTR = 1), but HTR was found to be insensitive to changes of proton energy above 20 MeV. As a result the relationship between HTR and relative TL efficiency is not unequivocal. The HTR was found to be dependent on absorbed dose even for the lowest studied doses.     

Dose response of F center optical absorption in LiF:Mg,Ti (TLD-100)

Optical absorption (OA) of nominally pure single crystal LiF following beta irradiation was measured in order to estimate, the energy and width of the dominant F-band with minimum interference from dopant-related bands. The OA dose response of LiF:Mg,Ti was measured to 30,000 Gy, a level of dose sufficiently high to observe total saturation of the F band, which, we believe, reduces uncertainty in the estimation of the dose filling constant. The dose filling constants for the OA bands associated with the trapping center (4 eV) and competitive center (5.45 eV) responsible for the major dosimetric TL glow peak 5 were also determined. The results of these studies will be used in the framework of a kinetic model which includes the effects of radiation created defects and which will aid in the investigation of the capability of Track Structure Theory to predict OA heavy charged particle (HCP) relative efficiencies.     

A study on thermal degradation of LiF:Mg,Cu,P and LiF:Mg,Cu,Si

We investigated the thermal degradation of LiF:Mg,Cu,P (NTL-250) and LiF:Mg,Cu,Si (MCS) for the development of TL sheet. By thermogravimetry and differential scanning calorimetry (TG-DSC), the exothermic reaction was observed between 320 °C and 400 °C in MCS as well as NTL-250. The heat value of MCS was twice as large as that of NTL-250. This ratio corresponded with that of Mg amount in these TL materials measured by ICP-OES (inductively-coupled plasma optical emission spectrometry). X-ray diffraction (XRD) measurements were also carried out, and the peaks of MgF₂ phase were also observed in degraded MCS sample as well as NTL-250. Moreover, X-ray absorption near-edge structures (XANES) of Cu in these LiF TLDs were measured. The valences of Cu did not change before and after degradation. It indicates that the thermal degradation is caused by not Cu but Mg ion state change. The exothermic reaction is possible caused by the stabilization reactions, and then it was expected to correspond with MgF₂ precipitation. From these results, we concluded that the thermal degradations of these LiF TLDs are caused by the precipitation of MgF₂.     

Application of phototransferred thermoluminescence (PTTL) for dose re-assessment in routine dosimetry using MTS-N (LiF:Mg,Ti) thermoluminescent detectors

Erasure of the thermoluminescence (TL) signal on detector readout is considered to be a disadvantage of TL dosimetry, as post-readout dose reassessment is then impossible in principle. A method of dose reassessment based on phototransferred thermoluminescence (PTTL) has been developed at the Institute of Nuclear Physics, Polish Academy of Sciences (IFJ PAN) and applied to MTS-N (LiF:Mg,Ti) detectors. We demonstrate the possibility of applying PTTL for dose reassessment in MTS-N TL detectors routinely applied in the dosimetric service at IFJ PAN. Readings of TL detectors exposed to relatively high doses by the customers of our dosimetry service can now be reassessed using our automatic readers. A major obstacle in applying the PTTL method at lower exposures is the presence of residual dose accumulated in LiF:Mg,Ti detectors after many field exposure and readout cycles. Since most of the TL detectors in our service have been already used for a long time (e.g. for over 10 years in the case of some detector batches), we find that our PTTL method of dose reassessment is possible only in detectors which had received doses exceeding 5 mSv.     

Study of Optically Stimulated Luminescence of LiF:Mg,Ti for beta and gamma dosimetry

Modern advances in radiation medicine – radiodiagnosis, radiotherapy and interventional radiography – each present dosimetry challenges for the medical physicist that did not exist previously. In all of these areas a constant balance has to be made between the treatment necessary to destroy the tumor and the unnecessary exposure of healthy tissue. Innovative applications of OSL dosimetry are now appearing in each of these areas to help the medical physicist and oncologist design the most effective, and least deleterious, treatment for their patients. High sensitivity, precise delivery of light, fast readout times, simpler readers and easier automation are the main advantages of OSL in comparison with TLD.This work aimed to study the application of OSL technique using lithium fluoride dosimeters doped with magnesium and titanium (LiF:Mg,Ti) for application in beta and gamma dosimetry.     

Investigation and simulation of the structural and electronic properties of LiF:Mg,LiF:Cu,LiF:P nano-layer dosimeters

In this study, electronic structure of lithium fluoride thin films in pure state and doped with magnesium (Mg), copper (Cu) and phosphorus (P) impurities was studied using WIEN2K Code. The structural and electronic properties of two LiF thin films with 1.61 and 4.05?nm thicknesses were studied and compared. Results show that the distance of atoms in the surface and central layers of pure LiF are 1.975 and 2.03?nm, respectively. Electronic density of the valence band around the surface atoms is greater than that around middle atoms of the supercell. The band gap of bulk LiF is 9?eV. But, in the case of thin films, it is reduced to 2?eV. Electronic and hole-traps were not observed in composition of LiF thin films doped with Mg and P with 1.61 and 4.05?nm thickness and in fact, metallic properties were observed. When Cu atoms were doped in composition of an LiF thin film, the thin film was converted to semiconductor.     

Kinetic simulation of charge transfer following 5.08 eV (F band) optical excitation of irradiated LiF:Mg,Ti (TLD-100): Participation of holes released via V3-VK transformation

Kinetic simulations of charge transfer in the framework of the conduction band/valence band model are described which investigate the effect of 5.08 eV photon bleaching on the optical absorption spectrum of irradiated LiF:Mg,Ti (TLD-100). The decrease in intensity of the 3.8 eV and 4.3 eV bands, newly discovered sub-entities of the 4.0 eV composite band, is interpreted as arising from the participation of holes released by capture of electrons at V₃ two-hole-centers. The simulations also require highly efficient electron transfer from the excited state of the F center to the V₃ center which is necessary to guarantee an adequate supply of released holes following the V₃-V_k transformation.     

Spectral characteristic of high-dose high-temperature emission from LiF:Mg,Cu,P (MCP-N) TL detectors

High-temperature emission spectra of LiF:Mg,Cu,P (MCP-N) TL detectors, irradiated above the nominal saturation level, up to the hundreds of kGy, have been measured. Emission spectra integrated over the whole temperature range, as well as the spectra recorded at the temperatures corresponding to the TL peaks maxima, were analyzed. With increasing dose of γ-radiation no significant changes were observed in the short wavelength emission range (220–450 nm) of the measured spectra. For doses of 4 kGy and higher the long wavelength emission (450–800 nm) started to be visible. All recorded spectra have been expressed in a form of the sum of several Gaussian-shape bands in the energy domain, which parameters remain in a general agreement with the measurements of Mandowska et al. (2010). Spectra of the low-temperature, main, high-temperature and “B” TL peaks were investigated. In the ranges of the low-temperature and the main dosimetric peaks, that is 100–125 and 210–230 °C, respectively, the short wavelength emission disappeared with increasing dose and for the highest doses the long wavelength emission became dominant. Both the high-temperature (290–320 °C) and the “B” (370–425 °C) peaks emission spectra exhibited somewhat different behavior with increasing dose. Initially, an even growth of the whole spectrum was observed and for doses higher than 16 kGy the intensity of the spectrum decreased, but the short wavelength emission band fell significantly faster, in case of the high-temperature TL peaks. In case of the “B” peak emission spectra the long wavelength emission did not play any role in the analyzed dose range. The spectra measured at the TL peaks maxima were also fitted with several Gaussian-shape bands. Dose-intensity dependences for all Gaussian-shape bands fitted to the measured spectra are also included in this paper.     

The effect of thermal annealing on defect structure and thermoluminescence in LiF:Mg,Cu,P

We have studied the behavior of the glow peaks in the thermoluminescence of LiF:Mg,Cu,P as a function of pre-irradiation annealing temperature in the range 80 to 170°C, and as a function of cooling rate following the 240°C/10 min anneal used for standardization in dosimetric procedures. The intensities of the major peaks in LiF:Mg,Cu,P (as well as in LiF:Mg,Ti—the current industrial standard) seem to be determined by the dynamics of clustering of (Mg²⁺−Li_vac) dipoles to dimers, trimers and a precipitate phase. The intensities of the thermal interactions, however, seem to be somewhat reduced in LiF:Mg,Cu,P compared to LiF:Mg,Ti. In addition, it seems plausible that phosphorus takes the role of titanium in LiF:Mg,Cu,P in the formation of a trapping center/recombination center spatially correlated complex.     

Nanodosimetric kinetic model incorporating localized and delocalized recombination: Application to the prediction of the electron dose response of the peak 5a/5 ratio in the glow curve of LiF:Mg,Ti (TLD-100)

A kinetic model combining both localized and delocalized recombination is described which is based on different filling rates as a function of irradiation electron energy of a spatially correlated trapping center/luminescent center (TC/LC) complex. Following irradiation and thermal de-trapping the locally trapped electron-hole configuration is assumed to give rise to peak 5a and the e-only configuration to peak 5 in the glow curve of LiF:Mg,Ti (TLD-100). The model is capable of simulating the linear/supralinear dose response of composite peak 5, the dependence of the supralinearity on photon energy and the ratio of the intensities of peak 5a to peak 5 as a function of dose. However, this is achieved only by invoking the presence of band-tail states which allow thermally induced hopping leading to semi-localized recombination in the recombination mechanism of the e-only configuration.