agation Protection Dosimetry Vol. 1 No, 3p. 153.167 [Nuclear Technology Publishing THERMOLUMINESCENCE DOSIMETRY AND ITS APPLICATIONS A. S, Pradhan Division of Radiological Protection, Bhabha Atomic Research Centre, Trombay, Bombay-400 085, India, Received Oct 1 1980, Revised July 10 1981, Accepted Sept 5 1981 Abstract—Thermoluminescence dosimetry (TLD) is generally recognised as a most versatile technique for the quantitative ‘measurement of X, gamma and beta radiations, especially in personnel monitoring. Developments in this field of radiation protection dosimetry are reviewed. In view of the trend of switching over to TLD by many personnel monitoring services the importance of the TLD system is discussed. The characteristics of some commercially available TLD systems and their associated problems are summarised. The usefulness of CaSO,:Dy detectors for X and gamma ray dose measurement is discussed, INTRODUCTION The credit of discovering thermoluminescence goes to Robert Boyle, who reported to the Royal Society in London, on Oct. 28, 1663, his observations of a strange “glimmering light”” on heating a diamond in thedark. Probably, Wiedemann (1895) wasthe firstto report the use of thermoluminescence from artificially prepared CaSO,:Mun for the detection of radiation due to an electrical discharge, and this method was again used by Lyman (1935) for measurements in the far ultraviolet range. Tousey et al (1951)0) used thermoluminescence for the measurement of UV and X-say radiations encountered during V-2 rocket flights. Randall and Wilkins in 1945 and Garlick and Gibson in 1949 provided a sound understanding of some aspects of the thermoluminescence process. The topic became a subject of comprehensive interest when its usefulness in radiation dosimetry was demonstrated in 1953 by Daniels et al, Thereafter Cameron et al proved the value of LiF from the Harshaw Chemical Co. USA for the measurement of X, gamma and beta rays and thermal neutrons. In the late sinties and seventies 2 major amount of work has been done in this field all over the world. Dosimetry methods based upon thermoluminescence detectors hhave many advantages in sensitivity, range, simplicity of reading, ruggedness, small size and potentially low cost. This hasattracted the attention of alarge number of investigators. THERMOLUMINESCENCE ‘Thermohuminescence (TL) is the phenomenon of light emission caused by heating a pre-irradiated TL material. TL dosemeters contain inorganic crystalline or polycrystalline materials doped with suitable activators. On the basis of investigations on the phenomenon (inchding optical absorption, ionic and photo-conductivity, electron spin resonance etc.) a number of models have been developed. They deal with some of the most conspicuous aspects and explain the behaviour to a limited degree. A very clear understanding of the TL mechanism has not yet been achieved. The TL sensitivity of a detector is the amount of light released per unit of radiation dose. The sensitivity ischaracteristic of a TL material and is. one of the main factors involved in determining its threshold detection limit. The location of the TL glow peak {peak on the pattern of light output versus temperature), and its size and shape, are influenced by the heating rate, radiation dose and pre- and post- irradiation heat treatments, whereas the emission spectrum (spectral distribution of the light at a given temperature) mostly depends on the nature of the activator. The glow peak temperature is usually an indicator of the rate of fading of stored information in a TL phosphor. However there exists no direct, relationship between peak temperature and fading rate, because there are many lattice parameters that influence TL stability; there have been cases of anomalous fading of very high temperature glow peakst®. At high temperatures the luminescence efficiency of some of the phasphors is also reduced. PROPERTIES OF TL DETECTORS Forradiation dosimetry itis preferable to havea TL detector with:- @ a simple glow curve structure (ideally a single slow peak around 200°C); Gi) ahigh gamma ray sensitivity: ii) negligible fading of TL signal on storage for a flew months at room temperature; 153,A.S, PRADHAN (iv) emission spectrum around 4500 A; (9) linear response (dose versus TL); (vi) simple annealing procedure for reuse Gasensitive to thermal history); (ii) chemical stability and inertness to extreme climatic variations ; (ill) effective Z close to that of tissue; ‘ix)_insensitivity to daylight. Table 1 summarises the important TL character- istics of some TL phosphors. LiF:(Mg,Ti)®, Mb, 0,:Dy®, Li,B,0,:Mn™, Li,B,0,:(Cu,Ag), 2Cu and “Beo!are among ‘te phosphors hakisg ow Z."The development of MgB,0,:Dy and Li,B,0,:Cu as highly promising TL phosphors has been reported recently®®. These phosphors are yet to become_available for dosimetric applications. The higher Z phosphors are CaF,:Dy™, CaF,:Ma, CaF natural}, Mg,Sidg Tot", CaSOy:Mnt's ALare, 18, CaSO:Tm” and CaS0¢By", Although in has the highest sensitivity, its stored information fades very rapidly and hence it is unnuitable for long term dose oessurements, Mg,Si0,:Tb, which is the next highest in TL. sensitivity, is sensitive to ultra-violet light. The post-irradiation fading of TL signal of some common phosphors when stored at various temperatures and relative humidities" is shown in Figure 1. Apart from temperature and humidity, the fading rate is also sometimes influenced by UV and daylight. The effect of light on the stability of gamma ray induced TL of some phosphors is shown in Figure 209, LiF (Mg, Ti) is perhaps the most widely used TL phosphor. The detector has been used widely in spite Of its several drawbacks, such as complicated peak structure (as many as 12 glow peaks) and structure is sensitive to thermal history), the need for sophisticated instrumentation for the measurement of low doses (~0.01 mGy), supralinearity beyond 10Gy, severe radiation damage beyond 10° Gy, and unknown preparation parameters. Recently, Johnson and Luersen have found that in LiF:(Mg, Ti), fading of dosimetric glow peaks is not the same for {ferent types of radiations due to a change in glow curve structure and transfer to higher energy traps. Further, in field conditions it has been found that LiF dosemeters may exhibit a high TL reading if contaminated with fine dust particles of highly sensitive thermoluminescent materials such as ALJ and CaF. However, LiF:Mg,Ti is still relered because of its lower effective 2, small fading rate, chemical inertness and commercial availability. Also this detector is valuable due to its availability in ferent isotopic compositions, such as ‘Li enriched TLD-600, "Li enriched TLD-700 and with natural Li abundance (TLD-100). These detectors with very different isotopic compositions have approximately the same gamma ray sensitivity, but have different sensitivities to neutrons; this makes LiF phosphors highly useful in mixed neutron-gamma fields. i.B,0,:Ma detectors are also used even though they ‘suffer from the drawbacks of temperature and humidity-dependent TL response and carly supralinearity; also the emission spectrum (around 6000A) does not match the peaking range of commonly-used photomultiplier tubes (around 4000 A). The main factor in favour of lithium borate has been its tissue equivalence. Among the currently available TL detectors, CaS0,:Dy does not suffer from the disadvantages discussed above and exhibits ‘good dosimetric properties except for its high photon energy dependent response below 100 keV. Also the Complications in reuse procedure (the glow curve preparation procedure of CaS0,;Dy is simple, and Table: General charsclerinis of some TLD phowphors Reaive Themision Desimetic Useful —_Efetive ‘Photon TL Signifeant mamma peakpeak vanee onic energy ‘aaine ‘effect TLD phosphor “ray emp, No-@ dependence ortigh sensitivity co aL30 keV in (eo=) enhancing ‘aainw Lirate.th 1 «ce Bs 42 13—«10%monh_———ON Mek oyDy 7 amoast00 210 = £413 0te/iwomomth Lipeonnia e400 Zo ormaywo cy 7.4098 0me/month No Tigbeoy Cae 5360 Suc wielGy T4889 NNmoMTh Yes & 580 23 7 Te Ose "Seetwormontm NO 32 4820 20 Gy toy 180 LS 0Ge/month No 3 aso0ast0 © 210 cyrolO'Gy 138.013 S/momh ON 70 $000, Ho fGyt0sOGy 50 La aotdny » 16 480045100200 Gio OSGy 160186 ADmonth Yes, 5 000 1m Kyte i8Gy 6D 1S Nmonth CorgNawa) 3800 20 1iGy to Wey 1k aS 7 a Mbi0g To 3 5520 15 Gyro ty 103 S/momih Yen Be 3.1 r000000 180-220 omeyioIOGy 7.2 Oa? Sehymonln Yes ‘Aly 5 290 2 IGy to Gy 12S Srtwowerks Yes Is4‘THERMOLUMINESCENCE DOSIMETRY 10 90 70 50°C,31 %RH 100 80 REL. DOSIMETER READING IN “h LigB,O7:Mn 40 2°497 20 20 40 60 70°C ° 20 STORAGE TIME (DAYS) ‘Figure 1. Fading of TL at various temperatures and relative humidities of different dosemeters. Post-irradiation annealing used for CaF,:Dy was 100°C/25 min and for other dosemeters 100°C/10 min. (After large batches of phosphor (each batch of 0.3 Ke) can ‘easily be prepared™. ‘The main dosimetric glow peaks of almost all the TL phosphors (Table 1) exhibit saturation for doses beyond 10’ Gy. However high temperature glow peaks® of some phosphors can still be used for high level gamma ray dosimetry. Caldas and Mayhugh®* have demonstrated that photo-transfer processes from high temperature glow peaks in phosphors such ‘as Ca50,:Dy can be used for dosimetry up to 10° Gy. Since it is preferable to have a sensitive but energy independent dosemeter, attempts have been made to 155 hart et, al} reduce the energy dependence of high Z and sensitive phosphors such as CaS0,:Dy by using sensitization?” (subjecting the TL phosphor to high gamma ray exposure followed by partial annealing). This reduces the energy dependence by about 30% due to the fact that there is an increase in TL sensitivity to low LET radiations, whereas the sensitivity to high LET radiations (low energy X-rays) is not much affected. This method has some drawbacks e.g. the sensitization is strongly dependent on pre-exposure ‘and the temperature of partial annealing, different batches of phosphors do not exhibit sensitization toA. 8, PRADHAN, 1.0 0-8 o - 06 w z z J 04 }O~CaFp:Dy = & A ~ Li,B,05Mn oe LY 7 Cafymn 0 ~ CaSO,Tm x- Bi pee ue 4 a 4 3 o «8 wf wh we wo 0 10 10% STORAGE TIME ( Min) Figure 2, Thermal fading of different TLD materials. Storage at 70°C, (a) in the dark, and (b) with access of daylight, (After Regular et alf20), the same degree, and the low level measuring capability of the phosphor is decreased due to unstable and increased TL background of the sensitized phosphor. ‘There have been suggestions to reduce the energy dependence by embedding the high 2 TL phosphors” in a low Z binding matrix. By this method the energy deposited in TL phosphor grains due to secondary electrons which originated in the binding material becomes significant compared to the energy deposited by the secondary electrons produced in the phosphor itself. The study of photon energy dependence of CaS0,:Dy embedded teflon TLD dises® hasshown that the dependence is not affected significantly by the proportion of phosphor in teflon for grain size ~74 um. This dependence could, however, be significantly reduced by embedding the phosphor of very low grain size ( = < a w a 2.0 1.0 10! 2 5 10? 2 7 10° PHOTON ENERGY (keV) Figure 4. Photon energy dependence of CaS0:Dy; (@), CaS0:Dy loose powder. (b), CaS0,Dy embedded teflon diss (0.8mm thick) containing 259% phosphor (grain size <75 am) by wi). PATIENT DOSIMETRY TLD has found extensive application in X-ray diagnosis and radiotherapy. The main advantage of TLD in medical applications are the availabilty of the detectors in various shapes and sizes, and the ease with which they may be attached to the skin. The dosemeters are found to be very convenient for monitoring cumulative dose, even in a hospital environment, and data can be obtained without significant disruption of physician or nursing routines”. Many surveys have been conducted to collect data on radiation doses to patients undergoing mammography”, dental radiography” and chest radiography. This has helped to obtain an idea of operating parameters, work practice and risk factors. In eye radiotherapy, TLD measurements have been frequently used to aid the design of protection shields” and to arrive at a proper position of patients to reduce the radiation dose to eye lenses, TLDs have also been used in many special cases in REFERENCES determining gonad dose during radiotherapy"). In. X-ray diagnostic radiography, since the radiation received by the skin of a patient undergoing X-ray investigation is a mixture (wide spectrum) of the primary beam and lower energy ra backscattered from tissue, the use of Li,B,0,:Mn has been recommended®. On the other hand some investigators have observed that even high Z detectors such as CaF," do not show significant variation in response in the diagnostic X-ray energy range. Some others have successfully used CaSO,:Dy for the measurement of entry, exit and gonad doses to patients undergoing mass miniature radiography”. Figure 4 shows the photon energy dependence of CaSO,:Dy detectors. 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