Lithium fluoride: from LiF:Mg,Ti to LiF:Mg,Cu,P

Differences and similarities between LiF-based LiF:Mg,Ti and LiF:Mg,Cu,P are discussed, with respect to their dosimetric properties--sensitivity, non-linearity of dose response and heavy charged particle efficiency, as related to the concentration and the individual role of the Mg, Ti, Cu and P dopants. To study further the role of these dopants, the properties of some new, 'hybrid' phosphors: LiF:Mg,Cu,Ti and LiF:Mg,P, specially developed for this purpose, are also discussed. In the glow curve of LiF:Mg,Cu,P with a low concentration of Mg a new peak was found, which appears to be an analogue of peak 4 in LiF:Mg,Ti, Magnesium apparently controls most of the dosimetric properties of LiF-based phosphors. For instance, charged-particle efficiency appears to be anti-correlated with the concentration of Mg, being much less dependent on the content of other dopants. On the other hand, some properties of LiF-based systems seem to be correlated with changes in the emission spectra. It is suggested that Ti hampers the acceptance of any increased amount of Mg into more traps in LiF:MgTi. The absence of Ti, not the presence of P or Cu, is therefore a key to the high sensitivity of LiF:MgCuP.     

Influence of readout parameters on TL response,re-usability and residual signal in LiF:Mg,Cu,P

It has recently been recommended that heating rates do not exceed 10 K.s(-1) and that the maximum temperature of readout should not exceed 265 degrees C for LiF:Mg,Cu,P. In some cases, a decrease of sensitivity in this material in the first of several re-use cycles had been reported. Influence of heating rates up to 30 K.s(-1), duration time up to 40s and maximum readout temperatures up to 270 degrees C on TL response, re-usability and residual signal was investigated. It was found that the maximum readout temperatures above 240 degrees C may lead to the thermoluminscent response decrease in the first several re-use cycles. The readout parameters can be optimised to minimise the residual signal (less than 0.4%) and to retain a constant sensitivity at the same time at high heating rates up to 30 K.s(-1) in a short time (less than 1 min per TL chip) without the necessity of heating above 240 degrees C. A concept of 'efficient residual signal' was put forward to quantify more accurately the real residual signal which affects the precision of the next measurement.     

Development of LiF:Mg,Cu,Si TL material (new KLT-300) with a low-residual signal and high-thermal stability

LiF-based thermoluminescence (TL) materials have been widely used for radiation dosimetry due to their attractive features. LiF:Mg,Cu,P is one of the most sensitive tissue-equivalent TL materials, approximately 40 times more sensitive than LiF:Mg,Ti (TLD-100), but it has two main drawbacks: a thermal loss of the TL sensitivity when annealed at temperatures >240 degrees C, and a relatively high-residual signal. Recently, LiF:Mg,Cu,Na,Si TL material was developed to overcome these drawbacks at the Korea Atomic Energy Research Institute, but it provided only marginal improvements in reducing the residual signal. The newly developed LiF:Mg,Cu,Si TL material has a significantly lower residual signal and a better stability to thermal treatments. In this article, the preparation method and some dosimetric properties (sensitivity and residual signal) of the new LiF:Mg,Cu,Si TL material are presented. At the end of the preparation procedures, a dual-step annealing method is introduced and this has proved as a very efficient method to reduce the high-temperature peak and is the cause of residual signal. Therefore, the high-temperature peak in the glow curve was significantly reduced. The sensitivity is approximately 20 times higher than that of TLD-100 and the residual signal was estimated to be approximately 0.04%.     

Sensitivity loss of Lif:Mg,Cu,P thermoluminescence dosemeters caused by oven annealing

LiF:Mg,Cu,P is a very sensitive thermoluminescence material that can be used for personal dosimetry in radiology. But if this material is heated too much during annealing or reading it quickly loses its sensitivity. This study shows that an annealing oven in wide use can cause thermal damage to the dosemeters owing to inhomogeneous temperature distribution in the annealing tray. At annealing temperatures>240 degrees C, differences of only 1 degrees C lead to significant losses of sensitivity. Therefore, it is necessary to measure the distribution of temperature in the annealing tray for correct placement of the dosemeters in the tray.     

Pre- and post-irradiation fading effect for LiF:Mg,Ti and LiF:Mg,Cu,P materials used in routine monitoring

LiF is a well-known thermoluminescent (TL) material used in individual monitoring, and its fading characteristics have been studied for years. In the present study, the fading characteristics (for a period of 150 d) of various commercial LiF materials with different dopants have been evaluated. The materials used in the study are those used in routine procedures by the Personal Dosimetry Department of Greek Atomic Energy Commission and in particular, LiF:Mg,Ti (MTS-N, TL Poland), LiF:Mg,Cu,P (MCP-N, TL Poland), LiF:Mg,Cu,P (MCP-Ns, thin active layer detector, TL Poland) and LiF:Mg,Cu,P (TLD100H, Harshaw). The study showed that there is a sensitivity loss in signal of up to 20 % for the MTS-N material for a 150-d period in the pre-irradiation fading phase. The MCP-N has a stable behaviour in the pre-irradiation fading phase, but this also depends on the readout system. As far as the post-irradiation fading effect is concerned, a decrease of up to 20 % for the MTS-N material is observed for the same time period. On the other hand, the LiF:Mg,Cu,P material presents a stable behaviour within ± 5 %. These results show that the fading effect is different for each material and should be taken into account when estimating doses from dosemeters that are in use for >2 months.     

The application of LiF:Mg,Cu,P to large scale personnel dosimetry: current status and future directions

LiF:Mg,Cu,P is starting to replace LiF:Mg,Ti in a variety of personnel dosimetry applications. LiF:Mg,Cu,P has superior characteristics as compared to LiF:Mg,Ti including, higher sensitivity, improved energy response for photons, lack of supralinearity and insignificant fading. The use of LiF:Mg,Cu,P in large scale dosimetry programs is of particular interest due to the extreme sensitivity of this material to the maximum readout temperature, and the variety of different dosimetry aspects and details that must be considered for a successful implementation in routine dosimetry. Here we discuss and explain the various aspects of large scale LiF:Mg,Cu,P based dosimetry programs including the properties of the TL material, new generation of TLD readers, calibration methodologies, a new generation of dose calculation algorithms based on the use of artificial neural networks and the overall uncertainty of the dose measurement. The United States Navy (USN) will be the first US dosimetry processor who will use this new material for routine applications. Until June 2002, the Navy used two types of thermoluminescent materials for personnel dosimetry, CaF2:Mn and LiF:Mg,Ti. A program to upgrade the system and to implement LiF:Mg,Cu,P, started in the mid 1990s and was recently concluded. In 2002, the new system replaced the LiF:Mg,Ti and is scheduled to start replacing the CaF2:Mn system in 2006. A pilot study to determine the dosimetric performance of the new LiF:Mg,Cu,P based dosimetry system was recently completed, and the results show the new system to be as good or better than the current system in all areas tested. As a result, LiF:Mg,Cu,P is scheduled to become the primary personnel dosimeter for the entire US Navy in 2006.     

UV-induced bleaching of deep traps in Harshaw TLD LiF:Mg,Cu,P and LiF:Mg,Ti

The effects of UV-induced bleaching of deep traps on Harshaw thermoluminescent (TL) LiF:Mg,Cu,P and LiF:Mg,Ti materials were investigated. During a normal heating cycle, LiF:Mg,Cu,P is limited to a maximum temperature of 240 °C. LiF:Mg,Ti can be read to higher temperatures; however, encapsulation in polytetrafluoroethylene limits the maximum readout temperature to 300 °C. Generally, for both materials, these respective temperatures are sufficient for emptying traps corresponding to the main dosemetric peaks. However, when the dosemeters are subjected to a high dose level, such as 1 Gy (much higher than individual monitoring dose levels), higher temperature traps are filled that cannot be emptied without exceeding the above-mentioned maximum temperatures. These high temperature traps tend to be unstable during normal readout and can significantly increase the residual TL signal. The purpose of this study was to investigate the applicability of a UV-induced bleaching technique for emptying higher temperature traps following high-dose applications. In addition, in the case of LiF:Mg,Cu,P, where the maximum readout temperature is significantly lower, we investigated the possibility of reducing the residual signal using the application of repeated readout cycles. The optical bleaching approach was found to be effective in the case of LiF:Mg,Ti; however, for LiF:Mg,Cu,P, no reduction in the residual signal was observed. For this latter material, the application of repeatable readout cycles is very effective and residual signals equivalent to dose levels as low as 0.01 mGy were observed following an initial dose of 5 Gy. To the best of our knowledge, this work is the first attempt to apply an 'optical annealing' technique to the Harshaw thermoluminescent dosemeter (TLD) materials.     

The application of computerised analysis of glow curves to personal dosimetry in LiF:Mg,Cu,P

In personnel monitoring services, it is important to omit the high-temperature annealing process so that large numbers of TL detectors can be produced economically. There are two efficient ways of reducing the residual signal of LiF:Mg,Cu,P. One is by increasing the maximum readout temperature and the other is by improving the preparation procedure (increasing the Cu concentration and the sintering temperature) but both reduce the TL sensitivity. In personal dosimetry the real dosimetric signals are separated from the residual signals by computerised analysis of glow curves. The adverse influence of the high residual signals of LiF:Mg.Cu.P TL material has been effectively eliminated and the sensitivity remains stable. A good dosimetric result using only reader measurement without pre-irradiation oven annealing is attained in a dose range of 50-80,000 microGy.     

Long-term fade study of the DT-702 LiF: Mg,Cu,P TLD

LiF thermoluminescent dosemeters (TLDs) are used by the US Navy to record radiation exposure of personnel. The Model DT-648 LiF:Mg,Ti TLD has been replaced by a new Model DT-702 LiF:Mg,Cu,P TLD. The DT-648 was used for many years and has undergone extensive testing to identify its pre- and post-irradiation fade operating characteristics. Studies have shown that the addition of copper increases the thermoluminesence sensitivity of the TLD for improved low-level radiation monitoring. This study evaluates various fading characteristics of the new copper-doped dosemeter using current equipment for processing of TLDs and calibrating to a National Institute of Standards and Technology standard source. The 57-week study took place at the Naval Dosimetry Center, Bethesda, MD, USA. TLDs were stored for various lengths of time before and after being exposed to a National Institute of Standards and Technology calibrated radiation sources. TLDs were then processed using current US Navy instructions and the resulting dose compared with the calibrated exposure. Both loss of signal and loss of sensitivity were evaluated. The results of this study have shown that the DT-702 TLD has no statistically significant change in sensitivity or change in signal with up to 57 weeks of pre- or post-irradiation time. The results of this study will increase the accuracy of exposure record keeping for the Navy and will allow longer issue periods. This will increase flexibility with international and domestic shipping procedures, as well as reduce workload requirements for dosimetry processing.     

TL emission spectra from differently doped LiF:Mg detectors

There are two widely applied types of thermoluminescent detectors based on LiF:Mg luminophor: Lif:Mg,Ti and highly sensitive LiF:Mg,Cu,P. The role of luminescence centres in these materials is usually attributed to defects connected with, respectively, titanium and phosphorus dopants. In order to check how composition of dopants introduced into the LiF lattice influences emission spectra, measurements on a series of variously doped LiF:Mg samples were performed. Apart from LiF:Mg,Cu,P and LiF:Mg,Ti detectors with different concentration of activators, an experimental sample being a kind of a 'hybrid' between both standard materials was also prepared. It was synthesised with concentrations of magnesium and copper identical to those used for LiF:Mg,Cu,P preparation. but instead of phosphorus it was doped with titanium (LiF:Mg,Cu,Ti). The measurements of the emission spectra were performed by using a liquid nitrogen cooled CCD 1024E detector with an SP150 spectrograph. During the measurements the samples were placed inside a cryostat in a vacuum. Resulting data were numerically deconvoluted for individual peaks with respect to the wavelength and the temperature. The glow curve shape of this material resembles that of LiF:Mg,Cu,P, while sensitivity is at the level of LiF:Mg,Ti. Preliminary results indicate that emission of the LiF:Mg,Cu,Ti sample is similar to that of LiF:Mg,Cu,P rather than to LiF:Mg,Ti, showing a maximum for wavelengths well below 400 nm.     

Comparison of the effects of exposure to light in Harshaw LiF:Mg,Ti and LiF:Mg,Cu,P

The response of thermoluminescence dosemeters (TLDs) to light, in various conditions, has been studied. TLD cards containing both conventional lithium fluoride (LiF:Mg,Ti) and the high-sensitivity material LiF:Mg,Cu,P were available, so permitting a comparison between the two types. Also available for the tests were Harshaw(TM) extremity EXT-RAD (LiF:Mg,Cu,P) dosemeters. The LiF:Mg,Ti body TLD cards and the EXT-RAD extremity dosemeters both showed some response to fluorescent light, while the LiF:Mg,Cu,P cards showed no significant response. It is therefore concluded that LiF:Mg,Cu,P body cards need no special precautions to protect them from the effects of light. For LiF:Mg,Ti cards and extremity dosemeters, effects are small, but steps to avoid excessive light exposure should be considered.     

Study of real time temperature profiles in routine TLD read out--influences of detector thickness and heating rate on glow curve shape

This paper reports the results of a study using a commercial routine read out system with non-contact hot nitrogen heating and linear heating gas profiles. Glow curves of LiF:Mg,Ti as well as LiF:Mg,Cu,P were analysed for different linear heating rates beta from 1 to 30 degrees K s(-1). Different thermoluminescent detectors (TLDs) of different thicknesses (0.38-0.90 mm) were studied and compared. By means of the application of CGCD program considering kinetic parameters of the used TL-material the analysis of the peak temperature of the individual TL peaks lead to the approximation of the real heating profile T(chip)(t) in the TL chip. The real heating profile deviates strongly from linearity and can be characterised by the solution of a differential equation T(chip)(t) = F [T(gas)(t)]. The model of this equation is discussed in the paper. The difference between gas and chip temperatures are heating rate and chip thickness dependent and reach values of up to 100 degrees C (for thick detectors and fast heating rates). Especially for LiF:Cu,P, knowledge of the real chip temperature is essential, since read out shall be performed at the highest possible temperature, without destroying the dosimetric properties of the material. On the basis of this work, an optimisation of the readout parameters for LiF:Cu,P is possible.     

On the roles of the dopants in LiF: Mg,Cu,Na,Si thermoluminescent material

In this paper, some results of the study on the roles of the dopants in the LiF:Mg,Cu,Na,Si thermoluminescent (TL) material that was developed at the Korea Atomic Energy Research Institute for radiation protection are presented. Although there have been many studies to investigate the roles of the dopants in LiF:Mg,Cu,P TL material in the TL process, there are some discrepancies in the understanding of the roles of Cu and P between various researchers. In case of LiF:Mg,Cu,Na,Si TL material, there are a few studies on the roles of the dopants. Three kinds of samples in each of which one dopant is excluded, and the optimised sample, were prepared for this study. The measurements and analysis of the three-dimensional TL spectra, based on the temperature, wavelength and intensity, and the glow curves for those samples are used in this study. The results show that Mg plays a role in the trapping of the charge carriers and Cu plays a role in the luminescence recombination process; however, the effect of Na and Si on the glow curve structure and the TL emission spectra is much less than that of Mg and Cu. It is considered that Na and Si each plays a role in the improvement of the luminescence efficiency.     

Pre-irradiation and post-irradiation fading of the Harshaw 8841 TLD in different environmental conditions

The pre-irradiation and post-irradiation fading of a commercially available LiF:Mg,Cu,P thermoluminescent detector (TLD)-the Harshaw 8841 TLD-have been assessed. The Harshaw 8841 TLD comprises three TLD-700H chips (99.7% 7LiF and 0.03% 6LiF by weight) and one TLD-600H chip (4.4% 7LiF and 95.6% 6LiF by weight). Pre-irradiation and post-irradiation fading were measured for storage times up to 164 d and three different storage temperatures (-8, 25 and 50 degrees C). Dosemeters were irradiated in a mixed photon-neutron field so that the fading behaviour of the photon and neutron signals could be studied. The TLD-700H and TLD-600H chips exhibited complex changes in sensitivity and signal that depended on storage time, storage temperature and the type of radiation to which the chips had been exposed. However, the magnitudes of these changes in sensitivity and signal were relatively small. TLD-600H and TLD-700H, therefore, exhibit good stability of sensitivity and signal.     

Evaluation of the performance of two LiF:Mg,Ti and LiF:Mg,Cu,P dosemeters for extremity monitoring

In this paper, the results aimed at assessing the performance of two varieties of LiF detectors (LiF:Mg,Ti and LiF:Mg,Cu,P) in photon fields relatively to reproducibility, detection threshold and angular dependence as defined in the ISO 12794 standard are presented. The fading properties and the limit of detection were also investigated for both materials. The results suggest that both LiF varieties are well suited for extremity monitoring. However, better fading properties of LiF:Mg,Cu,P when compared with LiF:Mg,Ti, combined with previous results relatively to energy dependence suggests that LiF:Mg,Cu,P dosemeters are better suited for extremity monitoring.     

A comparative study on the susceptibility of LiF:Mg,Ti (TLD-100) and LiF:Mg,Cu,P (TLD-100H) to spurious signals in thermoluminescence dosimetry

It is well known that spurious signals can occur in thermoluminescence dosimetry (TLD) whenever contaminants (i.e. dirt, oil, dust) are present on the surface of the TLD card or crystal during the read-out process. For TLD cards, the Teflon material can also contribute to the background noise and this contribution has been found to depend on the material's light absorption. These non-radiation-induced signals contribute to the total light output during TLD read-out and can lead to incorrect dosimetry especially for low-dose measurements such as personal dosimetry. However, these spurious signals are generally in the low-temperature channels and are mostly accompanied by abnormal glow curves. Most of the published reports dealing with this type of spurious TL signal are on the LiF:Mg,Ti (TLD-100) material. The relatively new TLD material, LiF:Mg,Cu,P, is more sensitive and has higher signal-to-noise ratio than the traditional LiF:Mg,Ti. In this study, the effects of disturbing signals to the LiF:Mg,Cu,P (TLD-100H) cards used in personal dosimetry are investigated and compared with those of LiF:Mg,Ti (TLD-100).     

Thermoluminescence properties of LiF:Mg,Cu,Na,Si pellets in radiation dosimetry

Sintered LiF:Mg,Cu,Na,Si thermoluminescence (TL) pellets have been developed for application in radiation dosimetry. LiF:M,Cu,Na,Si TL pellets were made from TL powders using a sintering process, that is, pressing and heat treatment. These pellets have a diameter of 4.5 mm, and a thickness of 0.8 mm are blue in colour and have a mass of 28 mg each. After 400 pellets had been produced they were irradiated with 137Cs gamma radiation and samples having a sensitivity within a +/-5% standard deviation were selected for experimental use. In the present study, the physical and dosimetric properties of LiF:Mg,Cu,Na,Si TL pellets were investigated for their emission spectrum, dose response, energy response and fading characteristics. Photon irradiation for the experiments was carried out using X ray beams and a 137Cs gamma source at the Korea Atomic Energy Research Institute (KAERI). The average energies and the dose were in the range of 20-662 keV and 10(-6) - 10(2) Gy respectively. The glow curves were measured with a manual type thermoluminescence dosimetry reader (system 310, Teledyne) at a constant nitrogen flux and a linear heating rate. For a constant heating rate of 5 degrees C.s(-1). the main dosimetric peak of the glow curve appeared at 234 degrees C, its activation energy was 2.34 eV and the frequency factor was 1.00 x 10(23). The TL emission spectrum appeared at the blue region centred at 410 nm. A linearity of photon dose response was maintained up to 100 Gy. The photon energy responses relative to the 137Cs response were within +/-20% in the overall photon energy region. No fading of the TL sensitivity of the pellets stored at room temperature was found over the course of a year. Therefore LiF:Mg,Cu,Na,Si TL pellets can be used for personal dosimetry, but more research is needed to improve the characteristics for repeated use.     

Time-resolved spectroscopy of LiF:Mg,Cu,P

Time-resolved spectroscopy measurements of LiF:Mg,Cu,P luminescence are presented to obtain a better understanding of the emission characteristics of this material. The intensities and decay of the emission bands were studied as a function of annealing temperature and ionising radiation (gamma) dose. Two peaks in the emission were observed at 367 and 466 nm when excited by the 266 nm laser radiation. The luminescence spectrum under band-to-band X-ray excitation shows a dominant emission approximately 390-400 nm, which resembles the reported thermoluminescence emission and is clearly different from the spectrum obtained using the 266 nm pulsed laser excitation. Annealing of the material to 300 degrees C increases the intensity of the 367 and 466 nm emission bands by an order of magnitude as well as changes the relative intensity of the bands. Additional emission bands, which are not evident in the thermoluminescence emission spectra, are seen at longer wavelengths that also increase with dose. Possible explanations for the observed emission spectra are discussed in this paper.     

Comparative study of LiF:Mg,Cu,Na,Si and Li2B4O7:Cu,Ag,P TL detectors

Recently, two new types of 'tissue equivalent' thermoluminescent detectors (TLDs) have aroused attention: LiF:Mg,Cu,Na,Si and Li2B4O7:Cu,Ag,P. In this work the characteristics of both detectors were compared with the characteristics of the well-known type LiF:Mg,Ti detector, TLD-100. The following properties were investigated: the glow curve structures, relative sensitivity, batch homogeneity and uniformity, detection threshold, reproducibility of the response, linearity in the wide dose range and fading. Also, the energy dependence for medium and low energy X rays was determined in the range of mean energies between 33 and 116 keV. The results confirmed 'tissue equivalency' of both new types in the investigated range of photon energies. LiF:Mg,Cu,Na,Si detector has very high sensitivity (approximately 75 times higher than that of TLD-100) and is convenient for use in a very low range of doses. Li2B4O7:Cu,Ag,P detector shows some improvements in comparison with the previously prepared types of lithium borate. The most important is the five times higher sensitivity than that of TLD-100. This detector is also very promising, especially in medical dosimetry.