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.     

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.     

High-dose characterization of different LiF phosphors

The dose response of three LiF TLDs: standard LiF:Mg,Ti (denoted MTS), high-sensitive LiF:Mg,Cu,P (MCP) and a recently developed in Kraków version of LiF:Mg,Ti with modified activator composition (MTT) and increased high-LET response was measured. The TLDs have been exposed to ⁶⁰Co gamma-rays, up to dose of 10 000 Gy, i.e. beyond saturation dose of the main dosimetric peaks, which corresponds to ca. 1000 Gy. The measured glow-curves were deconvolved into separate peaks with first order kinetic function (using self-developed GlowFit software). The dose response of the main peaks was found to be supralinear for MTS and sublinear for MCP detectors, as expected. The dose response of MTT was found to be even more supralinear than that of MTS. An interesting effect has been observed with regard to glow-curve shape of MCP detectors. Up to a dose of 1 kGy it remains practically unchanged, while for higher doses a strong growth of high-temperature peaks is observed. In the same dose region a decrease of the main peak of MCP with increasing dose is observed, unlike LiF:Mg,Ti detectors.     

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.     

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.     

Relative efficiency of TL detectors to energetic ion beams

The relative TL efficiency of LiF:Mg, Ti and LiF:Mg, Cu, P was evaluated for several ion beams, ranging from helium to xenon ions. Irradiations were realized at the HIMAC accelerator in Chiba, Japan, partly within the ICCHIBAN intercomparison project. The covered LET range was extending from about 2 keV/μm to 1500 keV/μm.Both tested TLD types exhibited a decrease of relative response with increasing ionization density – stronger for LiF:Mg,Cu,P detectors. The relationship between efficiency and LET was found to follow unique trend lines, as nearly all data points lied within 5% around the fitted empirical functions. Values of TL efficiency measured for various batches of same type TLDs agree within a few percent. The measured relationships between relative TL efficiency and LET will be used in the analysis of data obtained from space dosimetric experiments.     

Environmental gamma-ray dose rate measurement by using ultra-high sensitive LiF:Mg,Cu,Si TLD

Environmental gamma-ray dose rates were measured by using ultra-high sensitive LiF:Mg,Cu,Si thermoluminescence dosimeters (TLDs) during short-term burial. The resultant gamma-ray dose rates were compared with those measured by using optically stimulated luminescence (OSL) of Al₂O₃:C and assessed by using HPGe spectrometer. Regardless of the short-term burial and the change of environmental conditions as well as the mismatch of the effective atomic number (Z_eff) with the soil (mainly SiO₂), good agreement was observed between the doses measured by TLDs and OSL dosimeters or the assessed doses. LiF:Mg,Cu,Si TLD has been found to be an effective alternative for the measurement of environmental gamma-ray annual dose rates for use in optical dating.     

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.     

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.     

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.     

Performance comparison of OSLD (Al2O3:C) and TLD (LiF:Mg,Cu,P) in accreditation proficiency testing

The U.S. Navy uses a dosimetric system, which employs the LiF:Mg,Cu,P thermoluminescence dosimeters (TLDs), developed and produced by Thermo Fisher Scientific. Every two years, the Naval Dosimetry Center (NDC) performs proficiency testing to maintain its national accreditation. Since 2007, the U.S. Navy has also tested InLight Basic - OSLN Optically Stimulated Luminescence Al₂O₃:C dosimeters (OSLD) manufactured by Landauer. In 2011 and 2013, the Naval Dosimetry Center performed proficiency testing for both systems. Here we present a comparison of the performance of TLDs (LiF:Mg,Cu,P) and OSLDs (Al₂O₃:C) in five categories of proficiency testing. The testing included irradiation with photons, neutrons, beta particles and selected mixtures of these radiations. All irradiations were performed at the Pacific Northwest National Laboratory (PNNL). The delivered doses were not reported to the NDC. The official comparison of delivered and reported doses was conducted by PNNL in terms of dose bias and its standard deviation for each category of accreditation. In total, the NDC reported to the PNNL doses for 147 dosimeters of each type (TLD and OSLD). Both NDC tested dosimetric systems have passed established limits. The comparison of OSLD and TLD system performance in each category is discussed. Advantages and disadvantages of both systems are analyzed.     

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.     

Thermoluminescence of nanocrystalline LiF:Mg, Cu, P

Nanocrystalline LiF:Mg, Cu, P of rod shape (about 30-40 nm in diameter and 0.3-0.5 μm in length) has been prepared by the chemical co-precipitation method. Thermoluminescence (TL) and dosimetric characteristics of the nanocrystalline phosphor are studied and presented here. The formation of the material was confirmed by the X-ray diffraction (XRD). Its shape and size were also observed by transmission electron microscope (TEM). The TL glow curve of the nanocrystalline powder shows a single peak at 410 K along with four overlapping peaks of lesser intensities at around 570, 609, 638 and 663 K. The observed TL sensitivity of the prepared nanocrystalline powder is less than that of the commercially available “Harshaw TLD-700H hot-pressed chips” at low doses but it still around three times more than that of LiF:Mg, Ti (TLD-100) phosphor. The 410 K peak of the nanomaterial phosphor shows a very linear response with exposures increasing up to very high values (as high as 10 kGy), where all the other thermoluminesent dosimeters (TLD) phosphors show saturation. This linear response over a large span of exposures (0.1 Gy-10 kGy) along with negligible fading and its insensitivity to heating treatments makes the nanocrystalline phosphor useful for its application to estimate high exposures of γ-rays. The ‘tissue equivalence’ property of this material also makes it useful over a wide range of high-energy radiation.     

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 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.     

Spectrally resolved thermoluminescence of highly irradiated LiF:Mg,Cu,P detectors

Well known, widely applied high sensitive thermoluminescence (TL) detector LiF:Mg,Cu,P (MCP-N) was investigated. This paper analyses changes of the TL emission spectrum of MCP-N after irradiation with ultra high doses (up to 500 kGy). Spectral dependence of TL on dose is very complex especially in the region of very high doses (>1 kGy). As a general trend we found that the number of peaks increases with dose in the long-wavelength region indicating new types of recombination centres (RCs). Wavelength peak positions for increasing doses are quite stable. Only some of them show slight red-shift.     

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.