A system for rapid large-area monitoring of gamma dose rates in the environment based on MCP-N (LiF:Mg,Cu,P) TL detectors

One lesson learned from the Chernobyl accident was that the spatial distribution of far-field contamination was strongly non-uniform due to local variation of atmospheric conditions, such as wind direction, rain etc. An environmental monitoring system using highly sensitive thermoluminescent LiF:Mg,Cu,P (MCP-N) detectors has been completed and field-tested. The system consists of 3000 MCP-N detectors in 1000 TLD cards (three TLDs per card), two Mikrolab automatic TL readers, heating ovens, and specially developed software which includes a database for rapid evaluation of results. The main dosimetric parameters of MCP-N dosemeters, such as thermally-induced fading, light sensitivity, minimum detectable dose, self-dose, zero-dose, energy response up to 6-7 MeV, influence of annealing and readout conditions on detector stability, have been tested. About 100 locations over an area of about 15,000 km2 in the south of Poland were selected for measurements lasting from 4 days to 3 months. The kerma rates measured over a 4 day screening period agree well with kerma rates determined over a 75 day monitoring period. Results from short- and long-term exposure periods agree well with those performed using MTS-N (LiF:Mg,Ti) over southern Poland in 1985, before the Chernobyl accident. Thus, using the system based on MCP-N detectors, one is able simultaneously to monitor environmental radiation kerma rates at a large number of locations over periods of four days or less. Provided natural background kerma rates at selected monitoring points are available prior to the accident, the system can be applied to assess kerma rates rapidly in the environment, following a nuclear accident.     

Energy response of different types of RADOS personal dosemeters with MTS-N (LiF:Mg,Ti) and MCP-N (LiF:Mg,Cu,P) TL detectors

The photon energy response of different RADOS (Mirion Technologies) personal dosemeters with MTS-N (LiF:Mg,Ti) and MCP-N (LiF:Mg,Cu,P) thermoluminescence (TL) detectors was investigated. Three types of badges were applied. The irradiation with reference photon radiation qualities N (the narrow spectrum series), and S-Cs and S-Co nuclide radiation qualities, specified in ISO 4037 [International Organization for Standardization (ISO). X and gamma reference radiations for calibrating dosemeters and doserate meters and for determining their response as a function of photon energy. ISO 4037. Part 1-4 (1999)], in the energy range of 16-1250 keV, were performed at the Dosimetry Laboratory Seibersdorf. The results demonstrated that a readout of a single MTS-N or MCP-N detector under the Al filter can be used to determine Hp(10) according to requirements of IEC 61066 [International Electrotechnical Commission (IEC). Thermoluminescence dosimetry systems for personal and environmental monitoring. International Standard IEC 61066 (2006)] for TL systems for personal dosimetry. The new RADOS badge with the experimental type of a holder (i.e. Cu/Al filters) is a very good tool for identifying the radiation quality (photon energy).     

Microdosimetric interpretation of the photon energy response of LiF:Mg,Ti detectors

Photon energy response of MTS-N (LiF:Mg,Ti) detectors (TLD Poland) and of MTS-N detectors sensitised with 200 Gy of 60Co gamma rays, followed by UV irradiation (sMTS-N), has been determined using X rays with narrow energy spectra, in the energy range from 20 to 300 keV. The over-response of LiF:Mg,Ti detectors for X rays (relative TL efficiency eta = 1.1) can be explained as an ionisation density effect. Low energy X rays produce short electron tracks, which locally deposit a high radiation dose and, consequently, lead to an enhanced (supralinear) response. This over-response has not been observed in sensitised MTS-N where supralinearity in the response after gamma ray doses above 1 Gy is not seen. Using the dose-response curves measured for MTS-N detectors after 137Cs gamma ray irradiation and local doses calculated using Monte Carlo generated electron tracks, it was possible to predict the relative TL effectiveness for different X ray energies. The calculation procedure can be applied to predict the photon energy response of LiF:Mg,Ti detectors in an arbitrary photon field.     

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.     

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.     

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.     

The influence of post-exposure heating on the stability of MCP-N (LiF:Mg,Cu,P) TL detectors

Post-exposure annealing of highly sensitive LiF:Mg,Cu,P (MCP-N) detectors, at 100 degrees C over 10 or 20 min prior to readout, is usually recommended for routine dosimetry. The purpose of this anneal is to eliminate low-temperature peaks, especially peak 3, which fades at room temperature in about 3 months. However, as this annealing procedure does not entirely eliminate peak 3, 10% of its thermoluminescent (TL) signal still being readable, a fading correction must be applied. The aim of this work was to optimise the conditions of post-exposure treatment, i.e. its temperature and duration, in order to facilitate the use of MCP-N detectors in routine dosimetry. MCP-N detectors were annealed in standard conditions, i.e. at 240 degrees C over 10 min and exposed to a dose of 5 mGy (137Cs). For post-exposure annealing, six different temperatures between 100 degrees C and 150 degrees C and two time periods (10 and 20 min) were tested. TL glow curves were deconvoluted with the GCA code. A post-exposure anneal at 120 degrees C over 10 min was found to be optimal. Heating at this temperature eliminates 100% of the TL signal of peak 3, while maintaining the area and maximum intensity of the main peak 4 unchanged. In this case, no fading correction needs to be applied. Annealing at higher temperatures, up to 150 degrees C, results in a loss of peak 4 signal, and is therefore not recommended.     

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.     

MCP-N (LiF:Mg,Cu,P) TLDs for radon measurements with charcoal canisters

A method of measurement of radon concentration in air was developed, based on high-sensitivity LiF:Mg,Cu,P (MCP-N, TLD Poland) thermoluminescent detectors installed in charcoal canisters. The canisters were exposed typically for 72 h in a calibration chamber with a radon concentration ranging from 100 Bq x m(-3) to 87 kBq x m(-3). It was found that in these conditions the signal registered by the TL detectors was proportional to the 222Rn concentration and the lowest limit of detection (LLD) was at a level of 100 Bq x m(-3). The proposed method can be used in large-scale, multi-site surveys aimed at screening for high levels of indoor radon concentration or for measuring ground radon exhalation rates.     

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%.     

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.     

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.     

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.     

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.     

Energy response of LiF and Mg2SiO4 TLDs to 10-150 keV monoenergetic photons

Energy response of LiF:Mg,Ti, LiF:Mg,Cu,P and Mg2SiO4:Tb thermoluminescence dosemeters (TLDs) was measured in the range 10-150 keV for monoenergetic photons at SPring-8 of an 8-GeV synchrotron radiation facility. The photon beam was monitored by a parallel-plate free-air ionisation chamber calibrated with an uncertainty of 3%. Owing to the small dimension of the beam, a rotating holder was designed in order to irradiate TLDs uniformly. The measured responses of LiF to energy were approximately in agreement with the calculated dose absorption dependence in the soft tissue. However, two types of LiF TLDs presented the different luminescent responses to the photon energy. The response of LiF:Mg,Ti had a smooth curve, and that of LiF:Mg,Cu,P presented a local maximum at 30 keV and a local minimum at 100 keV. The Mg2SiO4:Tb response was nearly bone equivalent. Linearity of dose responses was also confirmed up to 2 Gy on each TL material.     

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).     

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.     

Role of impurities in the thermoluminescence of LiF:Mg,Cu,P

The thermoluminescent properties of lithium fluoride doped with magnesium, copper and phosphorous are reviewed. This material shows specific advantages over LiF (TLD-100) in that is has higher sensitivity, less energy dependence and no supralinear behaviour with dose. However, it suffers from an irreversible loss in sensitivity when heated above 270 degrees C. Possible causes for this loss in sensitivity are discussed and experimental results are shown that indicate potential roles for the Cu, P and O impurities in this process. The present work focuses on the understanding of the impurity contents, inclusions, cluster formation and valence changes in this material by using differential scanning calorimetry (DSC) and glow discharge mass spectroscopy (GDMS). This research concludes that phosphorus inclusions are formed and a valence change of the Cu ions occurs after annealing above 270 degrees C, which degrades the TL sensitivity of LiF:Mg,Cu,P phosphors. It is also shown that a high content of oxygen in the material and control of the oxygen content during processing are critical to maintaining the sensitivity of these phosphors.     

Self-indicating radiation alert dosemeter (SIRAD)

This paper reports initial attempts to apply a thermoluminescent (TL) reader with CCD camera to identify cases of static and dynamic exposure of personal dosemeters to doses relevant for radiation protection. Standard MTS-N (LiF:Mg,Ti) and MCP-N (LiF:Mg,Cu,P) TL pellets with diameter of 4.5 mm and thickness of 0.9 mm were used in a standard DOSACUS/RADOS personal dosimetry badge (holder). Pb, Cu and Al filters were installed instead of the standard Al 264 mg cm(-2) filters used in the RADOS badge. The badges were exposed statically and dynamically to X rays ranging from 28 keV (molybdenum anode) to 125 keV (tungsten anode) and to 137Cs (662 keV) gamma rays. The absorbed doses (in tissue) ranged from 20 to 100 mSv. Detectors were readout in the CCD reader and 2-D images were collected. The results obtained indicated that it was possible to identify the static, front exposure of the personal dosemeters equipped with Cu filter for doses >20 mGy for X rays up to 125 keV.     

Determination of LiF:Mg,Ti and LiF:Mg,Cu,P TL efficiency for X-rays and their application to Monte Carlo simulations of dosemeter response

The simulation of response of a new passive area dosemeter for measuring ambient dose equivalent H*(10) for photons has been performed using the Monte Carlo code MCNP and experimentally determined responses of LiF:Mg,Ti and LiF:Mg,Cu,P thermoluminescent (TL) detectors for hard-filtered X-ray spectra from 20 to 300 keV and for 137Cs and 60Co gamma radiation. Relative TL efficiency for both types of detectors, determined in experiments with bare detectors and similar Monte Carlo simulations, compared favourably with prediction of microdosimetric models for proposed microdosimetric target sizes in the range of 20-40 nm. The concluding verification experiment showed small deviations between measured and simulated dosemeter energy response values in the range of a few percent.