Intrinsic dosimetry: Elemental composition effects on the thermoluminescence of commercial borosilicate glass

Intrinsic dosimetry is the method of measuring total absorbed dose received by the walls of a container holding radioactive material. By considering this dose in tandem with the physical characteristics of the radioactive material housed within the container, this method can provide enhanced pathway information for interdicted radioactive samples. Thermoluminescence (TL) dosimetry was used to measure ionizing radiation dose effects on stock borosilicate glass. Differences in TL glow curve shape and intensity were observed for glasses from different geographical origins. The different TL signatures strongly correlated with the concentration of alkaline earth metals and the ratio of sodium to the total amount of alkali metal present in the borosilicate glass.     

New scheme for dual readout of dose in polycrystalline Li2B4O7 irradiated with synchrotron X-rays from Indus-2

A new thermoluminescent (TL) dosimeter readout scheme was developed which allows for the measurement of both the single incident dose and the accumulated dose from multiple irradiations, through a novel dual readout procedure. Undoped, Mn doped and Cu doped polycrystalline Li₂B₄O₇ pallets were irradiated by synchrotron X-rays from Indus-2 with different dose. Thermoluminescence glow curves were taken at various heating rates. Two glow peaks were observed in each sample. TL intensities of different samples were compared and it was found that TL counts are more in Cu doped Li₂B₄O₇ sample. TL counts under each peak were calculated and a fixed ratio for two peaks was obtained. A new method of reading out the two peaks separately was formalized, allowing for greater flexibility in the use of TL based personnel dose monitoring devices.     

Thermoluminescence sensitivity of daily-use materials

The thermoluminescence (TL) response of silicon-rich daily-use materials, namely charoite (silicate gemstone), Spanish dental crown, phone chip and Spanish glass has been investigated. All the samples previously characterised by means of X-ray diffraction, electron microscopy associated with energy-dispersion and wavelength-dispersive spectrometry and X-ray fluorescence exhibit a reasonable sensitivity to ionising radiation. The preliminary results, based on their TL properties, allow us to speculate that these materials could be potentially of interest in situations where conventional dosimetric systems are not available. The dose dependence of the 400 nm TL emission of the studied samples displays a very good linearity in the range of 0.1–10 Gy.     

Photon dosimetry methods outside the target volume in radiation therapy: Optically stimulated luminescence (OSL), thermoluminescence (TL) and radiophotoluminescence (RPL) dosimetry

Dosimetry methods outside the target volume are still not well established in radiotherapy. Luminescence detectors due to their small dimensions, very good sensitivity, well known dose and energy response are considered as an interesting approach in verification of doses outside the treated region. The physical processes of thermoluminescence (TL), radiophotoluminescence (RPL) and optically stimulated luminescence (OSL) are very similar and can be described in terms of the energy band model of electron-hole production following irradiation.This work is a review of the main dosimetric characteristics of luminescence detectors which were used in experiments performed by EURADOS Working Group 9 for in-phantom measurements of secondary radiation (scattered and leakage photons). TL LiF:Mg,Ti detectors type MTS-7 (IFJ PAN, Poland), types TLD-100 and TLD-700 (Harshaw), OSL Al₂O₃:C detectors type nanoDot™ (Landauer Inc.) and RPL rod glass elements type GD-352M (Asahi Techno Glass Coorporation) are described. The main characteristics are discussed, together with the readout and calibration procedures which lead to a determination of absorbed dose to water.All dosimeter types used show very good uniformity, batch reproducibility and homogeneity. For improved accuracy, individual sensitivity correction factors should be applied for TL and OSL dosimeters while for RPL dosimeters there is no need for individual sensitivity corrections.The dose response of all dosimeters is linear for a wide range of doses.The energy response of GD-352M type dosimeters (with Sn filter) used for out-of-field measurements is flat for medium and low energy X-rays.The energy dependence for TLDs is low across the range of photon energies used and the energy correction was neglected. A significant over response of Al₂O₃:C OSLDs irradiated in kilovoltage photon beams was taken into account. The energy correction factor f_en was calculated by using the 2006 PENELOPE Monte Carlo code.With suitable calibration, all dosimeter types are appropriate for out-of-field dose measurements as well as for the in-phantom measurements of radiotherapy MV X-rays beams.     

A thermoluminescence study of mineral silicates extracted from herbs in the dose range 0.5–5 Gy

The presence of silicates in many personal objects suggests their potential use at low dose as fortuitous dosimeter in an accidental radiological exposure, when conventional dosimetry is not available. The goal of the present work is the dosimetric characterization of mineral silicates extracted from the plant Hibiscus Sabdariffa L, known as Jamaica flower, in the dose range 0.5–5 Gy. By studying the radiation-induced signal in time, the temperature integration region between 210 °C and 250 °C was found to be the most stable and also reduced the effects of thermal fading in the dose reconstruction process; the dose response curve was linear between 0.5 Gy and 5 Gy. By checking the change in sensitivity after repeated exposures to ionizing radiations and to high temperature heating, no variation in the glow curve shape or peak intensities were detected. To eliminate a pre-existing background signal, all the characterization measurements were performed with aliquots “annealed” by a preliminary readout of the TL.     

Using the OSL single-aliquot regenerative-dose protocol with quartz extracted from building materials in retrospective dosimetry

We report on the application of the single-aliquot regenerative-dose (SAR) protocol to the optically stimulated luminescence signal from quartz extracted from fired bricks and unfired mortar in retrospective dosimetry. The samples came from a radioactive materials storage facility, with ambient dose rates of about 0.1 mGy/h. A detailed dose-depth profile was analysed from one brick, and compared with dose records from area TL dosemeters. Small-aliquot dose-distributions were analysed from the mortar samples; one associated with the exposed brick, and one from a remote site exposed only to background radiation. We conclude that unfired materials have considerable potential in retrospective dosimetry.     

TL and OSL dosimetric properties of Opal gemstone for gamma radiation dosimetry

In this work, the response of the natural material Opal was studied in relation to its thermoluminescence (TL) and optically stimulated luminescence (OSL), after exposure to the gamma radiation of a ⁶⁰Co source. The structure of the powdered Opal was verified using the X-ray diffraction, scanning electronic microscopy and energy-dispersive X-ray spectroscopy techniques. The material, in its stone form, was turned into powder and mixed to Teflon (also in powder) in three different concentrations, and then pellets were manufactured. The aim of this work was to evaluate the response of these pellets in high-doses of gamma radiation beams, and to observe their possible application as dosimeters, using the TL and OSL techniques. The dosimetric properties of the samples were analyzed by means of different tests, as: TL emission curves and OSL signal decay curves, reproducibility of TL and OSL response, minimum detectable dose, TL and OSL dose–response curves (5 Gy–10 kGy), and fading. The results obtained in this work, for the TL and OSL phenomena, demonstrated that the pellets of Opal + Teflon present an adequate performance e possibility of use as dosimeters in beams of high-dose gamma radiation.     

Characterization of ferric ions diffusion in Fricke gel dosimeters by using inverse problem techniques

Diffusion of ferric ions in ferrous sulfate (Fricke) gels represents one of the main drawbacks of some radiation detectors, such as Fricke gel dosimeters. In practice, this disadvantage can be overcome by prompt dosimeter analysis, and constraining strongly the time between irradiation and analysis, implementing special dedicated protocols aimed at minimizing signal blurring due to diffusion effects. This work presents a novel analytic modeling and numerical calculation approach of diffusion coefficients in Fricke gel radiation sensitive materials. Samples are optically analyzed by means of visible light transmission measurements by capturing images with a charge-coupled device camera provided with a monochromatic filter corresponding to the XO-infused Fricke solution absorbance peak. Dose distributions in Fricke gels are suitably delivered by assessing specific initial conditions further studied by periodical sample image acquisitions. Diffusion coefficient calculations were performed using a set of computational algorithms based on inverse problem formulation. Although 1D approaches to the diffusion equation might provide estimations of the diffusion coefficient, it should be calculated in the 2D framework due to the intrinsic bi-dimensional characteristics of Fricke gel layers here considered as radiation dosimeters. Thus a suitable 2D diffusion model capable of determining diffusion coefficients was developed by fitting the obtained algorithm numerical solutions with the corresponding experimental data. Comparisons were performed by introducing an appropriate functional in order to analyze both experimental and numerical values. Solutions to the second-order diffusion equation are calculated in the framework of a dedicated method that incorporates finite element method. Moreover, optimized solutions can be attained by gradient-type minimization algorithms. Knowledge about diffusion coefficient for a Fricke gel radiation detector is helpful in accounting for effects regarding elapsed time between dosimeter irradiation and further analysis. Hence, corrections might be included in standard dependence of optical density differences and actual, non-diffused, absorbed dose distributions. The obtained values for ferric ion diffusion coefficient are around 0.65 mm² h^?1, being in good agreement with previous works corresponding to similar Fricke gel dosimeter compositions. Therefore, more accurate 2D and 3D dose mapping might be attained, thus constituting valuable improvements in Fricke gel dosimetry, and parallely a high precision method of diffusion modeling and calculation has been developed.     

Retrospective and emergency dosimetry in response to radiological incidents and nuclear mass-casualty events: A review

This paper reviews recent research on the application of the physical dosimetry techniques of electron paramagnetic resonance (EPR) and luminescence (optically stimulated luminescence, OSL, and thermoluminescence, TL) to determine radiation dose following catastrophic, large-scale radiological events. Such data are used in dose reconstruction to obtain estimates of dose due to the exposure to external sources of radiation, primarily gamma radiation, by individual members of the public and by populations. The EPR and luminescence techniques have been applied to a wide range of radiological studies, including nuclear bomb detonation (e.g., Hiroshima and Nagasaki), nuclear power plant accidents (e.g., Chernobyl), radioactive pollution (e.g., Mayak plutonium facility), and in the future could include terrorist events involving the dispersal of radioactive materials. In this review we examine the application of these techniques in ‘emergency’ and ‘retrospective’ modes of operation that are conducted on two distinct timescales. For emergency dosimetry immediate action to evaluate dose to individuals following radiation exposure is required to assess deterministic biological effects and to enable rapid medical triage. Retrospective dosimetry, on the other hand, contributes to the reconstruction of doses to populations and individuals following external exposure, and contributes to the long-term study of stochastic processes and the consequential epidemiological effects. Although internal exposure, via ingestion of radionuclides for example, can be a potentially significant contributor to dose, this review is confined to those dose components arising from exposure to external radiation, which in most studies is gamma radiation.The nascent emergency dosimetry measurement techniques aim to perform direct dose evaluations for individuals who, as members of the public, are most unlikely to be carrying a dosimeter issued for radiation monitoring purposes in the event of a radiation incident. Hence attention has focused on biological or physical materials they may have in their possession that could be used as surrogate dosimeters. For EPR measurements, in particular, this includes material within the body (such as bone or tooth biopsy) requiring invasive procedures, but also materials collected non-invasively (such as clippings taken from finger- or toenails) and artefacts within their personal belongings (such as electronic devices of which smart phones are the most common). For luminescence measurements, attention has also focused on components within electronic devices, including smartphones, and a wide range of other personal belongings such as paper and other polymer-based materials (including currency, clothing, bank cards, etc.). The paper reviews progress made using both EPR and luminescence techniques, along with their current limitations.For the longer-established approach of retrospective dosimetry, luminescence has been the most extensively applied method and, by employing minerals found in construction materials, it consequently is employed in dosimetry using structures within the environment. Recent developments in its application to large-scale radiation releases are discussed, including the atomic bomb detonations at Hiroshima and Nagasaki, fallout from the Chernobyl reactor and atmospheric nuclear bomb tests within the Semipalatinsk Nuclear Test Site and fluvially transported pollution within the Techa River basin due to releases from the Mayak facility. The developments made in applying OSL and TL techniques are discussed in the context of these applications. EPR measurements with teeth have also provided benchmark values to test the dosimetry models used for Chernobyl liquidators (clean-up workers), residents of Semipalatinsk Nuclear Tests Sites and inhabitants of the Techa River basin.For both emergency and retrospective dosimetry applications, computational techniques employing radiation transport simulations based on Monte Carlo code form an essential component in the application of dose determinations by EPR and OSL to dose reconstruction problems. We include in the review examples where the translation from the physical quantity of cumulative dose determined in the sampled medium to a dose quantity that can be applied in the reconstruction of dose to individuals and/or populations; these take into account the source terms, release patterns and the movements of people in the affected areas. One role for retrospective luminescence dosimetry has been to provide benchmark dose determinations for testing the models employed in dose reconstruction for exposed populations, notably at Hiroshima and Nagasaki. The discussion is framed within the context of the well-known radiation incidents mentioned above.     

A study on the real-time radiation dosimetry measurement system based on optically stimulated luminescence

The optically stimulated luminescent (OSL) radiation dosimeter technically surveys a wide dynamic measurement range and a high sensitivity.Optical fiber dosimeters provide capability for remote monitoring of the radiation in the locations which are difficult-to-acoess and hazardous.In addition.optical fiber dosimeters are immune to electrical and radio-frequency interference.In this paper,a novel remote optical fiber radiation dosimeter is described.The optical fiber dosimeter takes advantage of the charge trapping materials CaS:Ce, Sm that exhibit OSL.The measuring range of the dosimeter is from 0.1 to 100 Gy.The equipment is relatively simple and small in size,and has low power consumption.This device is suitable for measuring the space radiation dose and also can be used in high radiation dose condition and other dangerous radiation occasions.     

Intrinsic dosimetry of glass containers used to transport nuclear materials: Potential implications to the fields of waste management and nuclear forensics

Thermoluminescence (TL) and Electron Paramagnetic Resonance (EPR) dosimetry were used to measure dose effects in borosilicate glass with time, from 10 min to 60 days following exposure to a dose of up to 100 Gy. TL and EPR results were consistent and performed similarly, with both techniques capable of achieving an estimated limit of detection of between 0.5 and 1 Gy. Three peaks were identified in the TL glow curve at roughly 110 °C, 205 °C, and 225 °C. The intensity of the 205 °C peak was the dominant peak over the time period of this study. The stability of all of the peaks with time since irradiation increased with their corresponding temperature and no significant variation was observed in the glow curve response to a specified total dose attained at different dose rates. The intensity of the 205 °C peak decreased logarithmically with time regardless of total dose. Based upon a conservative limit of detection of 3.3 Gy, a 100 Gy dose would still be detected 2.7E3 years after exposure. Here, we introduce the concept of intrinsic dosimetry, the measurement of the total absorbed dose received by the walls of a container containing radioactive material. The foreseen advantage of intrinsic dosimetry comes from considering the measured absorbed dose received by containers in concert with the characteristics (amount, type) of the source of that dose, the radioactive material contained within the walls of the container, in order to provide enhanced information about the history of an unknown sample in question. Three hypothetical scenarios are presented to introduce this method and to illustrate how intrinsic dosimetry might benefit the fields of nuclear forensics and waste management.     

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.     

TL, EPR and optical absorption in natural grossular crystal

Grossular is one of six members of silicate Garnet group. Two samples GI and GII have been investigated concerning their luminescence thermally stimulated (TL). EPR and optical absorption and the measurements were carried out to find out whether or not same point defects are responsible for all three properties. Although X-rays diffraction analysis has shown that both GI and GII have practically the same crystal structure of a standard grossular crystal, they presented different behavior in many aspects. The TL glow curve shape, TL response to radiation dose, the effect of annealing at high temperatures before irradiation, the dependence of UV bleaching parameters on peak temperature, all of them differ going from GI to GII. The EPR signals around g=2.0 as well as at g=4.3 and 6.0 have much larger intensity in GI than in GII. Very high temperature (>800 °C) annealing causes large increase in the bulk background absorption in GI, however, only very little in GII. In the cases of EPR and optical absorption, the difference in their behavior can be attributed to Fe³⁺ ions; however, in the TL case one cannot and the cause was not found as yet.     

掺Yb硅酸盐玻璃的热漂白性能研究

采用传统高温熔融法制备了掺Yb硅酸盐玻璃, 玻璃组成为 60SiO₂-12Al₂O₃-28CaO-1.0 mol%Yb₂O₃. 将玻璃分成两组, 一组经总剂量3 kGy的Co⁶⁰γ辐射源辐射, 另一组做空白对照. 然后测试了玻璃未辐射、辐射后及热漂白后的吸收谱和近红外发光谱. 实验结果表明: 一定的热处理会使得玻璃在辐射过程中产生的色心缺陷发生分解, 即辐射后的玻璃在300–900 nm波段的吸收系数显著地降低了, 在400 nm处未经辐射、经3 kGy辐射以及热漂白后的玻璃吸收系数分别是0.93, 2.9, 1.89 cm^-1. 另外, 玻璃的近红外发光强度明显增强, 在1028 nm处未经辐射、经3 kGy辐射以及热漂白后的玻璃近红外发光相对强度分别是588, 261, 436, 从而极大地改善了玻璃的光学性能. 所以一定的热处理可以使辐射后的玻璃产生热漂白的现象. 研究结果为进一步发展抗辐射玻璃材料提供了新的实验依据.     

Response of CaSO4:Dy phosphor based TLD badge system to high energy electron beams from medical linear accelerator and estimation of whole body dose and skin dose

Response of thermoluminescent dosimeter (TLD) badge based on CaSO₄:Dy phosphor to high energy electron beams from medical linear accelerators was simulated using FLUKA Monte Carlo code and experimentally verified. This study was carried out in order to determine the response of TL discs under different filter regions of the TLD badge and their ratios under different irradiation conditions in the energy range 6–20 MeV of high energy electron beams. It was found that the response of TL disc under metal filters of the TLD badge (D1) is always higher than the response of the TL discs under Polystyrene filter (D2) and open window (D3) and its response was found to decrease with increase in the energy of the electron beam. Estimation of whole body dose and skin dose including its error was carried out as an extension of the present study in case of accidental exposure of radiation worker to high energy electron beam.     

Bismuth silicate glass containing heavy metal oxide as a promising radiation shielding material

Optical and FTIR spectroscopic measurements and electron paramagnetic resonance (EPR) properties have been utilized to investigate and characterize the given compositions of binary bismuth silicate glasses. In this work, it is aimed to study the possibility of using the prepared bismuth silicate glasses as a good shielding material for γ-rays in which adding bismuth oxide to silicate glasses causes distinguish increase in its density by an order of magnitude ranging from one to two more than mono divalent oxides. The good thermal stability and high density of the bismuth-based silicate glass encourage many studies to be undertaken to understand its radiation shielding efficiency. For this purpose a glass containing 20% bismuth oxide and 80% SiO₂ was prepared using the melting–annealing technique. In addition the effects of adding some alkali heavy metal oxides to this glass, such as PbO, BaO or SrO, were also studied. EPR measurements show that the prepared glasses have good stability when exposed to γ-irradiation. The changes in the FTIR spectra due to the presence of metal oxides were referred to the different housing positions and physical properties of the respective divalent Sr²⁺, Ba²⁺ and Pb²⁺ ions. Calculations of optical band gap energies were presented for some selected glasses from the UV data to support the probability of using these glasses as a gamma radiation shielding material. The results showed stability of both optical and magnetic spectra of the studied glasses toward gamma irradiation, which validates their irradiation shielding behavior and suitability as the radiation shielding candidate materials.     

Investigation of emission spectra,dose response and stability of luminescence from NaCl

The thermoluminescence (TL) from common salt (NaCl) is investigated to determine its suitability as an opportunistic retrospective dosimeter. In this study the TL is analysed from a wide range of domestic salts, sourced from Australasia, Europe, Asia and America. The emission spectra for pre-existing or “Natural” TL (NTL) and laboratory-irradiated “Artificial” TL (ATL) were analysed using a Fourier Transform spectrometer, giving luminescence intensity as a function of temperature and photon energy. Fading behaviour in the candidate TL emission peaks, observed at 200–260 °C under the measurement conditions used, was investigated at various storage temperatures and storage intervals between irradiation and read-out. This included TL emission spectral measurements at storage intervals ranging from minutes to months. Nearly all samples showed strong ATL emission at 590 nm, with much weaker emission from the commonly measured UV-blue region. NTL was very small or undetected for most samples. The storage tests showed that the TL in the 260 °C region is relatively stable and we conclude that TL from NaCl possesses suitable dose sensitivity and stability for use as an opportunistic retrospective dosimeter.     

Radiation-Induced Defects in Calcium Aluminate Glasses

In this work, MgF₂ and CaF₂ doped calcium aluminate glass samples have been investigated in order to describe the intrinsic defects that are formed in UV irradiated glasses. It is well known that calcium aluminate, when UV-illuminated, changes colour from blue to green. Thermoluminescence (TL), Optical Absorption (OA) and Electron Paramagnetic Resonance (EPR) measurements have been carried out and the results obtained were associated with the structural properties of the CaO—Al₂O₂—SiO₂ system, in order to provide a defect model. Thermal treatments up to 150°C were performed for OA and TL measurements but the thermal decay curves could not be adjusted by an exponential function. The TL experimental results were fitted, according to a continuous model, with a Gaussian distribution function centred at 0.6eV and a frequency factor of 10⁹s^?1.     

Thermoluminescence characterization of functionalized grafted polymers and its application for radiation dosimetry at low doses

Functionalized polymers were prepared by radiation-induced graft copolymerization of binary monomer system acrylic acid/acrylamide (AAc/AAm) onto low-density polyethylene (LDPE) and polypropylene (PP) films using direct radiation-grafting technique. Sulfonation was carried out for the prepared grafted copolymers using concentrated sulfuric acid (97%) at 60 ^°C for 15 min. The grafted and sulfonated grafted films found to have good properties such as thermal stability and hydrophilic properties. The sulfonated grafted films found to have a better hydrophilic character than the grafted ones due to ionic character resulted by this conversion. The thermoluminescence (TL) characteristics of a set of grafted and sulfonated films have been studied with regard to their use as off-line dosimeters in radiotherapy. The structural characterization has been performed by means of infrared spectroscopy. Their TL responses have been tested with radiotherapy beams of ⁶⁰Co photons in the dose range 0.1–7 Gy. The dosimetric characterization has yielded a very good reproducibility and is independent of the radiation energy. The TL signal is not influenced by the dose rate and exhibits a very low thermal fading. Moreover, the sensitivity of the samples compares favorably with that of the standard TLD100 dosimeters. Finally, at the same dose, the TL response for LDPE-g-P (AAm/AAc) films is higher than the PP-$g$-P(AAm$/$AAc), and the sulfonated grafted films are more sensitive to radiation than the grafted ones.