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.     

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.     

The effect of pre-irradiation annealing on the thermoluminescence of LiF:Mg,Cu, P phosphor grown by EFG technique

LiF crystal doped with magnesium (Mg), copper (Cu) and phosphorous (P) was grown in the form of multicrystalline sheet using Edge-defined film-fed growth (EFG) technique for dosimetry application. These crystals were grown in argon gas atmosphere using graphite crucible and stainless steel die. Dosimetry peak was observed at 210 °C for as-grown crystal. As reported earlier LiF:Mg, Cu, P is a highly sensitive material but losses its sensitivity if annealed at temperature above 240 °C. In this paper, the effect of annealing temperature on thermoluminescence glow-curve structure, maximum peak temperature, peak height and integrated area of the glow peak of EFG grown samples was investigated in detail. Annealing temperature range from 220 °C to 500 °C was considered for the study. Experimental results of the obtained glow curve show that with increase in annealing temperature, glow peak shift towards higher temperature region with substantial increase in TL intensity. Annealing at 500 °C for 10 min gave maximum TL intensity with main dosimetry peak positioned at 233 °C. Change in the defect structure with different pre-annealing temperature was analysed using trapping parameters.     

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.     

Further study on the influence of thermal treatments on the glow curve structure in LiF:Mg,Cu,P (GR-200A)

The influence of various annealing treatments with heating temperatures (T_A) from 240 to 700 °C, with re-annealing at 240 °C, and with a combined re-annealing procedure of 20 min at 270 °C followed by 10 min at 240 °C on LiF:Mg,Cu,P (GR-200A) was investigated. As the T_A increased, the intensity decreased rapidly to almost no signal at 340–380 °C then increased clearly and achieved a maximum at 540 °C. The position of the maximum intensity of the glow curve shifted basically in the direction of higher temperatures with an increase at T_A and achieved a maximum of 279 °C when annealed at 460 °C. The re-annealing influenced both the intensity and the glow curve structure at certain degree. The effect of re-annealing on the glow curve depended markedly on the T_A. With re-annealing at 240 °C, the intensity decreased as T_A increased up to 360 °C then increased and achieved a maximum at 540 °C. The intensity could be restored fully when annealed at above 500 °C, however, the glow curve couldn't be restored fully. With a combined annealing, the shape of glow curve of a sample annealed at above 540 °C or below 320 °C was similar to that of the standard glow curve of LiF:Mg,Cu,P and the intensity and glow curve could be restored completely when annealed in the range 620–660 °C. It seems that the main roles of the re-annealing at 240 °C are to restore partially the intensity of peak 4 and peak shape for LiF:Mg,Cu,P when annealed at above 260 °C, and restore fully the total TL intensity of LiF:Mg,Cu,P when annealed at above 500 °C and the main roles of the combined re-annealing are to reduce the intensity of peak 5 and the total TL intensity, increase the intensity of peak 4 and restore the glow curve shape.     

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 reusability characteristics of LiF:Mg,Cu,P with a maximum intensity at 280 °C in an environment with elevated temperature

Efforts are aimed at finding a method that could serve TL dosimetric measurements in the range of low-dose but carried out in an environment with elevated temperature. The temperature at the position of the maximum intensity of LiF:Mg,Cu,P was about 280 °C when annealed at 460 °C. LiF:Mg,Cu,P with a maximum intensity at 280 °C should present good thermal stability. The TL intensity of LiF:Mg,Cu,P with a maximum intensity at 280 °C was about 54% of the standard LiF:Mg,Cu,P, it should have a minimum measurable dose in the range of micro-Gy. LiF:Mg,Cu,P with a maximum intensity at 280 °C could be re-used by the 660 °C/30 min annealing, followed by 270 °C/20 min, 240 °C/10 min and 460 °C/30 min. It's possible for LiF:Mg,Cu,P to be extended application for low dose test in an environment with elevated temperature.     

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.     

Synthesis and thermoluminescence characterization of MgB4O7:Gd,Li

Magnesium tetraborate (MTB) doped with rare earth elements were synthesized by solid state sintering technique. Among the different rare earth dopants studied in this phosphor, gadolinium doped phosphors resulted in a single intense dosimetric peak at 250 °C and this is the first report in rare earth-doped MgB₄O₇ with a glow peak above 200 °C Photoluminescence (PL) and thermoluminescence (TL) studies were performed with this phosphor after exposing the powder samples to ionizing radiation. Monovalent dopants, including Na, Li and Ag, were found to increase the TL sensitivity of the MgB₄O₇:Gd phosphor without a shift in the TL peak temperature. The TL emission spectra showed characteristic emission of the host lattice, which showed an increase on doping with rare earth or monovalent codopants. The TL sensitivity, dose response curve, and post-irradiation storage stability were studied for the possible use of this material in radiation dosimetry applications. The TL parameters, such as the activation energy, the frequency factor, and the order of kinetics were determined for the Gd-doped MgB₄O₇ phosphor. The phosphor was found to be reusable after a few cycles of irradiation and annealing. The post-irradiation storage stability studies showed that this near tissue-equivalent phosphor, which has a gamma sensitivity five times that of TLD-100, is suitable for medical dosimetry applications.     

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.     

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.     

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.     

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.     

TL and EPR studies of CaSO4:Dy phosphor to investigate its efficacy in measurement of food irradiation dose at sub-ambient temperatures

The effects of sub-ambient temperatures of irradiation and dose response of CaSO₄:Dy phosphor was investigated. The irradiation dose in the range 0.5–7.0 kGy was chosen to meet the requirement of commercial food irradiation at low temperature. Commercially available phosphor showed no significant change in glow curve structure with low temperature of irradiation. In order to enhance the sensitivity of the low temperature glow peak (142 °C), the phosphor was subjected to different post-preparation thermal treatments at 700–900 °C. The change in glows and improvement in dose response characteristics were explained by Electron Paramagnetic Resonance (EPR) spectroscopy. At sub-ambient temperature of irradiation, the behavior of thermally treated CaSO₄:Dy phosphor with increasing dose revealed improved linear response of the low temperature glow peak and could be an efficient dosimetry system for the food commodities irradiated at low temperatures.     

Synthesis and thermoluminescence characterization of Na6Mg(SO4)4:RE (RE = Ce,Tb) phosphors

Thermoluminescence (TL) properties of sulfate-based phosphors activated by different rare earths have received tremendous attention to the field of radiation dosimetry. Those TL materials based on CaSO₄ have been widely applied for medical and environmental dosimetry. Taking this fact into account we have synthesized Na₆Mg(SO₄)₄ doped with Ce and Tb by wet chemical method. The prepared phosphor was characterized by XRD, FTIR, photoluminescence (PL) and thermoluminescence. For TL study, the phosphor is irradiated with γ-rays from ⁶⁰Co source. For studying luminescence properties, the prepared phosphor was annealed at different temperatures and effects of these annealing temperatures on Na₆Mg(SO₄)₄ samples are investigated and quantified. The changes in the glow curve and PL emission spectrum are also investigated as a function of annealing temperature and the annealing temperature was optimized. For calculation of trapping parameters various methods such as peak shape (PS) method, initial rise (IR) method, various heating rate (VHR) method, and computerized glow curve deconvolution (CGCD) are employed.     

Behaviour of LiF:Mg,Cu,P and LiF:Mg,Ti thermoluminescent detectors for electron doses up to 1 MGy

The behaviour of LiF:Mg,Cu,P and LiF:Mg,Ti detectors at ultra-high doses up to 1 MGy, has been investigated. The presence of the ultra-high-temperature peak (450 °C) of reproducible properties was observed in various batches of LiF:Mg,Cu,P, confirming earlier findings. The results indicate that this peak is not an effect of random impurities nor intrinsic effects of LiF, but it is rather connected with the doping.A parameter called ultra-high temperature ratio (UHTR) was defined in order to quantify the observed changes of LiF:Mg,Cu,P glow-curve shape at very high doses and very high temperatures. The use of this parameter allows to determine an absorbed dose in the range from 1 kGy to 1 MGy. This new method of high-dose dosimetry makes LiF:Mg,Cu,P a unique dosimeter, which is capable to cover at least 12 orders of magnitude of dose range: from a microgray to a megagray.     

Effects of annealing and high radiation dose on the thermoluminescence characteristics of natural fluorite

In this study, the various dosimetric properties of the thermoluminescent (TL) phosphor of CaF₂:natural including response characteristics, sensitivity to thermal annealing and decay of stored energy were investigated in detail. The analysis of the peak temperature values and the half widths of the resolved components in the glow curves, by using the Computerized Glow Curve Deconvolution (CGCD) Method, resulted in the activation energy (E) of 0.85–1.83 eV and frequency factor (s) of 6.17E+9–2.90E+15 s^?1. The effects of pre-irradiation thermal annealing on the radiation-induced sensitization of the thermoluminescent response of CaF₂:natural were presented. An enhancement of sensitivity after being subjected to a high beta particle exposure was clarified. The effect was complicated by the influence of heat treatments before the exposure to radiation. Replicate runs on CaF₂:natural after irradiation with 1 Gy absorbed dose indicated good reproducibility of peak temperatures and intensities; they can be re-used for repeated measurements. It appeared that the main dosimetric peak at 280 °C exhibits negligible fading over 4 weeks and may be used for dosimetry. This study has demonstrated that the potential exists for the use of CaF₂:natural for TL radiation dosimetry.     

Synthesis and luminescence properties of nanocrystalline LiF:Mg,Cu,P phosphor

Nanocrystalline LiF:Mg,Cu,P phosphor material of different shapes and sizes (microcrystalline cubic shape, nanorod shape and nanocrystalline cubical shaped) have been prepared by the chemical co-precipitation method. Thermoluminescence (TL) and other dosimetric characteristics of the phosphor are studied and presented here. The formation of the materials was confirmed by the X-ray diffraction (XRD). Its shapes and sizes were also observed using scanning electron microscope (SEM). The TL glow curve of the microcrystalline powder shows a prominent single peak at 408 K along with another peak of lesser intensity at around 638 K. On the contrary, the nanocrystalline rod shaped particles show a peak of low intensity at 401 K and a prominent peak around 700 K while the nanocrystalline particles in cubical shapes again show two peaks, one at around 407 K and the other at around 617 K, of which the lower temperature (407 K) peak is more prominent. The glow curve structure changes at very high doses (100 kRad) and some new peaks appear at around 525 and 637 K also the first peak appearing at around 401 K becomes prominent. The observed changes in TL due to the change in the shape and sizes of the nanophosphor have been reported. The PL has also been studied and various excitation and emission peaks observed due to the presence of various impurities are explained. The observed results have been explained in the light of asymmetrical crystal field effects due to asymmetrical shapes of the nanocrystalline phosphor. The comparison of these properties with the microcrystalline material prepared by the same co-precipitation method is also done.     

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.