RECENT DEVELOPMENTS IN COMPUTERISED ANALYSIS OF THERMOLUMINESCENCE GLOW CURVES: SOFTWARE CODES, MECHANISMS AND DOSIMETRIC APPLICATIONS.

The computerised deconvolution of thermoluminescence glow curves into component glow peaks is discussed in detail with special emphasis on advances of the subject post 2013. A plethora of computer codes have been developed using models based on first-order kinetics, second-orders kinetics, interactive traps and continuous distributions of activation energies. The glow curves of several materials are displayed and discussed along with new and improved dosimetric applications:precision effects of heating rate, heavy charged particles, mixed field α/ϒ dosimetry, fading and dose-response linearity. Finally recommendations are made for future efforts.

KINETIC SIMULATIONS OF THE THERMOLUMINESCENCE CHARACTERISTICS OF LIF:MG, TI INCORPORATING LOCALISED AND DELOCALISED RECOMBINATION.

Kinetic simulations of the thermoluminescence characteristics of LiF:Mg, Ti are reviewed in the framework of conduction band/valence band models. Delocalised recombination models have been mainly applied to the simulation of glow peak shapes, although comparison with experimental data has proven difficult if not impossible due to the scarcity of materials with demonstrably proven 'single-peak' glow curves. The delocalised models are incapable of the simulation of TL dose response linear/supralinear behaviour and the dependence of the supralinearity on particle energy. These characteristics require the incorporation of localised, nanodosimetric, recombination processes in the TL mechanisms. These investigations have simulated many of the TL characteristics of LiF:Mg, Ti in kinetic models based on a mixture of both delocalised and localised recombination.

RELATIVE HCP THERMOLUMINESCENCE AND OPTICAL ABSORPTION EFFICIENCIES: THE DEMISE OF TRACK STRUCTURE THEORY.

The thermoluminescence relative efficiency, ηTST, of LiF:Mg,Ti and LiF:Mg,Cu,P following heavy charged particle irradiation is calculated using track structure theory and compared with experimental measurements. The calculations use both 60Co generated values of secondary electron dose response and values of the dose response at lower photon energies. In both materials there is poor agreement with experiment. Optical absorption relative efficiencies are also in disagreement. For the F band, ηexpt'l/ηTST = 2.0 and 2.6 for He ions and protons, respectively. The values of ηexpt'l/ηTST for the 4.0-eV band, resulted in 0.18 (protons) and <0.12 (He ions). An indication that the 4.0-eV trapping structure is either destroyed or de-populated during the heavy charged particle (HCP) slowing down. The large deviations of ηexpt'l/ηHCP from unity demonstrate that TST, which predicts HCP induced radiation effects from the exclusive action of the released secondary electrons, is woefully inadequate.

DEMONSTRATION OF THE POTENTIAL AND DIFFICULTIES OF COMBINED TL AND OSL MEASUREMENTS OF TLD-600 AND TLD-700 FOR THE DETERMINATION OF THE DOSE COMPONENTS IN COMPLEX NEUTRON-GAMMA RADIATION FIELDS.

The results reported herein demonstrate the potential application of combined optically stimulated luminescence/thermoluminescent (OSL/TL) measurements in neutron-gamma discrimination dosimetry. The advantages of OSL/TL are two-fold: (i) The OSL and TL readout can be carried out on the same sample and (ii) the greater efficiency of OSL to high ionization density radiation due to F 2 and F3 excitation. The gamma/electron calibration coefficients for LiF:Mg, Ti (TLD-600 and TLD-700) were measured using a 90Sr/90Y source calibrated at the SARAF-SSDL nuclear facility. The estimation of the neutron calibration coefficients was carried out by irradiation with broad-spectrum beam of fast neutrons with median energy 5 MeV at the Radiological Research Accelerator Facility (RARAF) of Columbia University. Naturally cooled samples of TLD-600 and TLD-700 were dosed to levels of 29.8 Gy neutrons and 6.1 Gy gammas in air and KERMA calculations employed to transfer the levels of dose to6,7LiF. A figure of merit for fast-neutron/gamma ray discrimination was determined at 10.6 for TLD-700 in the current measurements. The use of combined TLD-600/TLD-700 allowed, as well, the determination of a considerable and somewhat unexpected thermal neutron component of 116 Gy in TLD-600.

DOSE DEPENDENCE OF RADIATION INDUCED DAMAGE IN THE THERMOLUMINESCENT RESPONSE OF LIF:Mg,Ti (TLD-100).

The effect of previous irradiation on the sensitivity of the glow peaks of LiF:Mg,Ti (TLD-100) is investigated up to levels of dose of 400 Gy in both slow-cooled and naturally cooled materials following the 400°C/1 hour pre-irradiation anneal. It is demonstrated that the naturally cooled samples can be re-used up to accumulated levels of dose of 50 Gy without recalibration. At 400 Gy a significant decrease in sensitivity of approximately 25% is observed for all the glow peaks (excluding peak 3). In slow-cooled materials even 100 Gy does not alter the sensitivity of the material.

MANIPULATION OF THE DOSE-RESPONSE OF COMPOSITE GLOW PEAK 5 IN THE THERMOLUMINESCENCE OF LiF:Mg,Ti (TLD-100) VIA OPTICAL EXCITATION POST-IRRADIATION: POTENTIAL FOR IMPROVED DOSE-RESPONSE LINEARITY BEYOND 1 Gy.

Many dosimetric applications and especially those involved in clinical dosimetry are hampered by the supralinearity of TLD-100 which begins at a level of dose of 1 Gy. This research investigates the effect of optical excitation following irradiation on the dose-response. It is expected that this will lead to a more linear dose-response, however, irrespective of the hoped-for linearity, the theoretical/kinetic simulations of the effect of optical excitation will further enhance our understanding of the thermoluminescence mechanisms, especially the role of spatially correlated trapping and luminescent centers. In the following, the various stages carried out in these investigations are discussed and preliminary results presented.

OSL and TL in LiF:Mg,Ti following alpha particle and beta ray irradiation: application to mixed-field radiation dosimetry.

The optically stimulated luminescence (OSL) of LiF:Mg,Ti (TLD-100) following irradiation by beta and alpha particles was investigated by the measurement of the excitation and emission spectra of OSL and comparison with thermoluminescence (TL) characteristics. Measurements were also carried out on nominally pure LiF monocrystals. The preferential excitation of OSL compared to TL following high-ionisation density (HID) alpha irradiation is naturally explained via the identification of OSL with the 'two-hit' F2 or F3+ centre, whereas the major component of composite TL glow peak 5 is believed to arise from a 'one-hit' complex defect. This discovery allows near-total discrimination between HID radiation and low-ionisation density radiation and may have significant potential in mixed-field radiation dosimetry.

Investigation of the ionisation density dependence of the glow curve characteristics of LIF:MG,TI (TLD-100).

The dependence of the shape of the glow curve of LiF:Mg,Ti (TLD-100) on ionisation density was investigated using irradiation with (90)Sr/(90)Y beta rays, 60 and 250 kVp X rays, various heavy-charged particles and 0.2 and 14 MeV neutrons. Special attention is focused on the properties of high-temperature thermoluminescence; specifically, the behaviour of the high-temperature ratio (HTR) of Peaks 7 and 8 as a function of batch and annealing protocol. The correlation of Peaks 7 and 8 with average linear-energy-transfer (LET) is also investigated. The HTR of Peak 7 is found to be independent of LET for values of LET approximately >30 keV microm(-1). The behaviour of the HTR of Peak 8 with LET is observed to be erratic, which suggests that applications using the HTR should separate the contributions of Peaks 7 and 8 using computerised glow curve deconvolution. The behaviour of the HTR following neutron irradiation is complex and not fully understood. The shape of composite Peak 5 is observed to be broader following high ionisation alpha particle irradiation, suggesting that the combined use of the HTR and the shape of Peak 5 could lead to improved ionisation density discrimination for particles of high LET.

The thermoluminescence dose-response and other characteristics of the high-temperature TL in LiF:Mg,Ti (TLD-100).

Various characteristics of the high-temperature thermoluminescence (HTTL) in the glow curve of LiF:Mg,Ti (TLD-100) are reviewed. The proposed applications of the HTTL to mixed-field radiation dosimetry are outlined with special emphasis on the question of the linearity/supralinearity of the HTTL dose-response at low dose levels from 2.5 to 250 mGy. Recent measurements of the HTTL dose-response using non-linear hot-gas heating and linear planchet heating are discussed in detail. It appears that a mild HTTL supralinearity of approximately 15-50% for each dose decade may be present, followed by an abrupt and rapid increase in the supralinearity >250 mGy. However, difficulty in the estimation of background and the great variability in the protocols of measurement do not allow a definitive conclusion. There is much work to be done in the areas of protocol standardisation, materials selection, methods of data analysis and especially the details of background behaviour, and subtraction before the HTTL can become a reliable dosimetric tool.

Ionisation density effects following optical excitation in LiF:Mg, Ti (TLD-100).

The TL signal following 5 eV photon excitation of previously irradiated and readout material has been studied as a function of ionisation density and various experimental parameters: (i) maximum temperature of the first readout; (ii) photon fluence; (iii) photon energy and (iv) beta ray dose. Following alpha particle irradiation, the ratio of the second-readout to first-readout TL signal, epsilon(alpha,) has been found to be 10-20 times higher than that following beta irradiation, indicative of the possibility of using the double ratio epsilon(alpha)/epsilon(beta) as a mixed-field discriminator. The beginning of an attempt to explain this unusual effect is offered in the framework of the track structure theory and kinetic modelling of the beta ray dose-response of the first and second readouts.

The effects of ionisation density on the glow curve structure of LiF:Mg,Ti (TLD-100): the behaviour of composite glow peak 5 in 'slow-cooled' material.

The effects of ionisation density on the structure of the glow curve of LiF:Mg,Ti (TLD-100) are briefly reviewed and discussed within the framework of the spatially correlated TC/LC model and localised recombination. The effects of 'slow-cooling' on the structure of composite peak 5 following low-ionisation density beta/gamma irradiation are described and analysed in both 'slow-cooled' and 'normally cooled' samples. It is demonstrated that 'slow-cooling' using a cooling rate of 30 degrees C h(-1) increases the relative intensity of glow peak 5a to composite glow peak 5 from approximately 0.1 to approximately 2, thereby greatly improving the precision of measurement of the ratio 5a/5. The improved precision removes a hurdle impeding the development of the ionisation density discrimination properties of the peak 5a/5 nanodosimeter.

Advanced multistage deconvolution applied to composite glow peak 5 in LiF:Mg,Ti (TLD-100).

The effects of 'slow-cooling' on the structure of composite peak 5 following low-ionisation density beta/gamma irradiation are described and analysed in both 'slow-cooled' and 'normally-cooled' samples. Computerised glow curve deconvolution is employed with constrained 'peak-shape' parameters deduced from anciliary studies using 4 eV and 5 eV optical excitation.

Theories of TL systems: failures, successes, conflicts, trends: insights into possible future materials and techniques.

In this paper some of the many theoretical models dealing with characteristics of TL materials are discussed. Special attention is given to some of the models dealing with the effects of ionisation density, that is Modified Track Structure Theory (MTST) and Microdosimetric Track Structure Theory (MTT) for the calculation of Heavy Charged Particle relative TL efficiencies, as well as solid-state models based on conduction band/valence band theory. Failures, successes, conflicts and trends are highlighted as well as a peek into future avenues of research for dosimetric TL materials.

Modelling the dose response of peaks 4, 5 and 5b, in TLD-100, as a function of recombination temperature.

This investigation focuses on whether the experimentally observed changes, in supralinearity f(D) as a function of recombination temperature, can be, successfully, predicted by the Unified Interaction Model (UNIM). To resolve this question, the measurement of f(D) has been carried out for glow peaks 4, 5 and 5b in LiF:Mg,Ti (TLD-100) at two different heating rates and UNIM analysis is used in an attempt to arrive at a consistent/physically reasonable explanation of all the f(D)/heating rate data for the three glow peaks. It is demonstrated that in addition to the variation in the luminescence and competitive centre capture cross section with temperature changes in the ks (the geminate recombination coefficient) parameter as a function of temperature is also required in order to predict the changes in f(D).

Theoretical and experimental investigation of the f(D)max-(S/S0)max anomaly in LiF:Mg,Ti.

Previous investigations in the framework of the Unified Interaction Model (UNIM) have demonstrated the difficulty in theoretically predicting both f(D)max and [S(Ds)/S(0)]max with the same set of UNIM parameters. This anomaly is re-investigated and an alternative explanation, based on experimental measurements combined with UNIM analysis, is given. This explanation is based on the assumption that N(LC), the total number of available luminescent centres is changed by the sensitisation dose or anneal or both. Allowing N(LC) to increase as the sensitisation dose is increased, a good fit to both f(D) and S(Ds)/S0 is obtained.

Properties of the 4.45 eV optical absorption band in LiF:Mg,Ti.

The optical absorption (OA) and thermoluminescence (TL) of dosimetric LiF:Mg,Ti (TLD-100) as well as nominally pure LiF single crystal have been studied as a function of irradiation dose, thermal and optical bleaching in order to investigate the role of the 4.45 eV OA band in low temperature TL. Computerised deconvolution was used to resolve the absorption spectrum into individual gaussian bands and the TL glow curve into glow peaks. Although the 4.45 eV OA band shows thermal decay characteristics similar to the 4.0 eV band its dose filling constant and optical bleaching properties suggest that it cannot be associated with the TL of composite peaks 4 or 5. Its presence in optical grade single crystal LiF further suggests that it is an intrinsic defect or possibly associated with chance impurities other than Mg, Ti.

Optical excitation of LiF:Mg,Ti following alpha and beta irradiation.

It is demonstrated experimentally that optical excitation of irradiated LiF:Mg,Ti (TLD-100) by 4 eV photons has the same effect for both alpha particle (high-ionisation density) irradiation and photon/electron irradiation. In both cases, peak 5a converts to peak 4 causing peak 4 to increase following the bleach. Such an observation is consistent with the major premise of track structure theory that radiation effects following heavy changed particle (HCP)/neutron irradiation are due exclusively to the interaction of the secondary electrons created by the HCP slowing down.

Search for ionisation density effects in the radiation absorption stage in LiF:Mg,Ti.

Optical absorption (OA) dose-response of LiF:Mg,Ti (TLD-100) is studied as a function of electron energy (ionisation density) and irradiation dose. Contrary to the situation in thermoluminescence dose-response where the supralinearity is strongly energy-dependent, no dependence of the OA dose filling constants on energy is observed. This result is interpreted as indicating a lack of competitive process in the radiation absorption stage. The lack of an energy dependence of the dose filling constant also suggests that the charge carrier migration distances are sufficiently large to smear out the differences in the non-uniform distribution of ionisation events created by the impinging gamma/electron radiation of various energies.

KINETIC SIMULATIONS OF THERMOLUMINESCENCE DOSE RESPONSE: LONG OVERDUE CONFRONTATION WITH THE EFFECTS OF IONISATION DENSITY.

The reader will time-travel through almost seven decades of kinetic models and mathematical simulations of thermoluminescence (TL) characteristics based on the band-gap theory of the solid state. From post-World-War II, ideas concerning electron trapping mechanisms to the highly idealised one trap-one recombination (OTOR) model first elaborated in 1956 but still in 'high gear' today. The review caresses but purposely avoids in-depth discussion of the endless stream of papers discussing the intricacies of glow peak shapes arising from first-order, second-order, mixed-order and general-order kinetics predominantly based on non-interacting systems, and then on to the more physically realistic scenarios that have attempted to analyse complex systems involving ever greater numbers of interacting trapping centres, luminescent centres and non-luminescent centres. The review emphasises the difficulty the band-gap models have in the simulation of dose response linear/supralinear behaviour and especially the dependence of the supralinearity on ionisation density. The significance of the non-observation of filling-rate supralinearity in the absorption stage is emphasised since it removes from consideration the possibility of TL supralinearity arising from irradiation stage supralinearity. The importance of the simultaneous action of both localised and delocalised transitions has gradually penetrated the mindset of the community of kinetic researchers, but most simulations have concentrated on the shape of glow peaks and the extraction of the glow peak parameters, E (the thermal activation energy) and s (the attempt-to-escape frequency). The simulation of linear/supralinear dose response and its dependence on ionisation density have been largely avoided until recently due to the fundamental schism between the effects of ionisation density and some basic assumptions of the band-gap model. The review finishes with an in-depth presentation and discussion of the most recent nanoscopic-localised/delocalised kinetic model that promotes an ice-breaking solution to bridge the schism.

The modified unified interaction model: incorporation of dose-dependent localised recombination.

The unified interaction model (UNIM) was developed to simulate thermoluminescence (TL) linear/supralinear dose-response and the dependence of the supralinearity on ionisation density, i.e. particle type and energy. Before the development of the UNIM, this behaviour had eluded all types of TL modelling including conduction band/valence band (CB/VB) kinetic models. The dependence of the supralinearity on photon energy was explained in the UNIM as due to the increasing role of geminate (localised recombination) with decreasing photon/electron energy. Recently, the Ben Gurion University group has incorporated the concept of trapping centre/luminescent centre (TC/LC) spatially correlated complexes and localised/delocalised recombination into the CB/VB kinetic modelling of the LiF:Mg,Ti system. Track structure considerations are used to describe the relative population of the TC/LC complexes by an electron-hole or by an electron-only as a function of both photon/electron energy and dose. The latter dependence was not included in the original UNIM formulation, a significant over-simplification that is herein corrected. The modified version, the M-UNIM, is then applied to the simulation of the linear/supralinear dose-response characteristics of composite peak 5 in the TL glow curve of LiF:Mg,Ti at two representative average photon/electron energies of 500 and 8 keV.