Potential use of wallboard (drywall) for EPR retrospective dosimetry

Concern regarding the possibility of criminal or terrorist use of nuclear materials has led to an interest in developing the capability to measure radiation dose in a variety of natural and manufactured materials. Electron paramagnetic resonance (EPR) measurements of radiation dose following a radiological incident may aid in screening affected populations (triage) and in reconstruction of doses following accidents. One such EPR dosimeter is wallboard (drywall), a common construction material composed largely of gypsum (calcium sulphate dihydrate). We have identified the CO₃⁻ and SO₃⁻ dose-sensitive lines in drywall and developed a measurement protocol using the intensity of CO₃⁻ line. Proper background subtraction is a major difficulty, and we demonstrate a procedure based on alignment of a contaminant Mn²⁺ line. As a proof-of-concept, a wallboard panel was irradiated with a ⁶⁰Co source, and a two-dimensional map of the absorbed dose was measured. While most aliquots yielded reasonably accurate doses, a spatially contiguous region of apparent dose-insensitivity in one panel was identified.     

On the use of OSL of chip card modules with molding for retrospective and accident dosimetry

The potential of optically stimulated luminescence of wire-bond chip card modules with molded encapsulations for retrospective and accident dosimetry is investigated. Contact-based and contactless modules were studied, the latter finding potential use in electronic documents (e.g. electronic passports, electronic identity cards). Investigations were carried out on intact as well as chemically prepared modules, extracting the filler material. Contact-based modules are characterized according to zero dose signal, correlation between OSL and TL, dose response and long-term signal stability. For prepared modules, the minimum detectable dose immediately after irradiation is 3 mGy and between 20 and 200 mGy for contact-based and contactless modules, respectively. Dose recovery tests on contact-based modules indicate that the developed methodology yields results with sufficient accuracy for measurements promptly after irradiation, whereas a systematic underestimation is observed for longer delay times. The reasons for this behaviour are as yet not fully understood.     

Luminescence from NaCl for application to retrospective dosimetry

The alkali halide NaCl (Common salt) is an environmentally-abundant phosphor of considerable potential for retrospective dosimetry and radiological event analysis due to its high sensitivity to ionising radiation when analysed by Thermoluminescence (TL), Optically-stimulated luminescence (OSL) or Infrared-stimulated luminescence (IRSL). We report here aspects of luminescence from NaCl relevant to the development of valid protocols for measurement of recent ionising radiation exposure. The timescale of interest in this application is from days to decades, hence our emphasis is on detection and characterisation of TL emission in the 100–300 °C range, and of OSL and IRSL emissions measured following only low temperature preheating (160 °C). A collection of 19 salt samples was assembled, including samples of rock salt and domestic salt produced by evaporation from brine. Analysis of TL emission spectral changes, together with previously reported TL, OSL and IRSL sensitivity changes, confirmed activation of sensitivity change by exposure to temperatures exceeding 160 °C. Kinetic analysis using Chen's method found E = 0.943 eV and s = 5.1 × 10¹¹ s^?1 for the 100 °C TL peak, giving a lifetime at 20 °C consistent with previous calculations and in the range of 7–14 h.     

New luminescence measurement facilities in retrospective dosimetry

This paper gives a review of recent developments in luminescence measurement facilities on the Risø TL/OSL reader including radio-luminescence (RL), exo-electron and violet stimulation attachments, and a method for characterising and if necessary correcting for beta irradiation source non-uniformity.We first describe improvements to the existing RL option to allow near infra-red detection (NIR) during irradiation by the built-in ⁹⁰Sr/⁹⁰Y beta source. The RL optical signal is collected by a liquid light guide through an F34-901 interference filter and detection is based on a dedicated thermoelectrically cooled NIR sensitive PMT (detection window peak at 855 nm, FWHM 27 nm). Software and electronics have been modified to allow standard TL and OSL measurements in the same sequence as RL measurements. Together with a new bleaching source based on a high-power UV LED (395 nm; 700 mW/cm²), this facility has been used to measure natural doses in feldspar using the decaying NIR RL signal.Secondly, we present a method for mapping radiation field of the built-in ⁹⁰Sr/⁹⁰Y β-source and estimating grain-location specific dose-rates. This is important for the accuracy of single grain results, when radiation field is spatially non-uniform across the sample area. We document the effect of this correction method and further investigate on the effect of lifting the source to achieve a better dose-rate uniformity.Finally we summarise two recently-developed novel facilities to help investigate (i) the time scales involved in OSL processes (time-resolved exo-electron detection) and (ii) extending the age range (violet stimulated signals from deep quartz OSL traps).     

Simulations of the predose technique for retrospective dosimetry and authenticity testing

The predose technique of thermoluminescence (TL) for quartz has been used extensively for retrospective dosimetry and archaeological authenticity testing. In this paper, we use a previously published comprehensive kinetic model for quartz, to simulate the complete sequence of experimental steps taken during the additive dose and the multiple activation versions of the predose technique. The simulation results show how both versions of the predose technique can reproduce the paleodose received by the sample with an accuracy of 1–5% in the low dose region of 0–2 Gy. For doses greater than $\sim 2\mathrm{Gy}$ the non-linear dose dependence of the sensitivity of the “$110{}^{\circ }\mathrm{C}$” TL peak causes significant inaccuracies in the technique. The solution of the kinetic differential equations elucidates several electron and hole processes taking place during the experimental predose procedure; these processes include the thermal transfer of holes from the Zimmerman hole reservoirs to the luminescence center, the radiation quenching of the TL sensitivity and the radiation-enhanced sensitivity of quartz samples. Specific numerical examples are given for samples exhibiting the thermal activation characteristics of “low-$S_0$” and “high-$S_0$” values. Quantitative results are presented for the effect of the test dose and of the calibration beta dose $\beta$ on the accuracy of both versions of the predose technique. Results are also presented for the sensitivity of the predose technique to the natural variations of the hole concentrations in the luminescence center. Finally, the results of the predose technique simulations are compared with those from simulating the popular single aliquot SAR/OSL technique based on optically stimulated luminescence signals.     

Luminescence properties of common glasses for application to retrospective dosimetry

Seventeen domestic and scientific glass specimens were investigated for thermoluminescence (TL) properties suitable for application to retrospective population dosimetry. Usefulness for retrospective dosimetry was initially judged by the presence of well-defined TL glow peaks and the absence of irradiation-independent luminescence. Of particular interest were TL glow peaks having relatively low trap depths, to prevent significant natural dose accumulation. Minimum useful trap lifetimes would be in the order of weeks. Surveys were undertaken to observe the TL and optically stimulated luminescence (OSL) behaviour of each sample. Most samples showed identifiable TL, with Pyrex in particular, and samples from a jar, a lampshade, and opaque blue beads all showing well-defined TL glow peaks with sensitivities that were not significantly affected by prior irradiation and heating of the sample. Kinetic analysis of these samples showed that their TL emission originates from traps with suitable stability for retrospective dosimetry. It is concluded that, while some glass samples show promising results, the inherent variability of an amorphous substance such as glass means that the suitability of each sample must be determined on a case-by-case basis.     

The zone strong coupling two-channel totally asymmetric simple exclusion processes

This article investigates the zone strong coupling two-channel totally asymmetric simple exclusion processes (TASEPs). The study is based on Pronina and Kolomeisky’s work [J. Phys. A-Math. Gen. 37, 9907 (2004)], in which the coupling exists within two whole parallel channels. Zone strong coupling two-channel TASEPs focuses on the behavior and the effect of a particular segment rather than the whole channel. The study shows that there are five possible stationary phases; LD/LD, HD/HD, MC/LD, LD/HD, and MC/HD. The phase diagrams and the density profiles are investigated using computer Monte Carlo simulations and mean-field approximation. The outcomes of the simulations match agreeably with the analytical predictions.     

Study of TSL and OSL properties of dental ceramics for accidental dosimetry applications

Interest is increasing in the development of new methodologies for accidental dose assessment, exploiting the luminescence and dosimetric properties of objects and materials which can be usually found directly on exposed subjects and/or in the contaminated area.In this work, several types of ceramics employed for dental prosthetics restoration, including both innovative materials used as sub-frames for the construction of the inner part of dental crowns (core), and conventional porcelains used for the fabrication of the external layer (veneer), were investigated with regard to their thermally and optically stimulated luminescence (TSL and OSL respectively) properties, in view of their potential application in accidental dosimetry.The sensitivity to ionizing radiation proved to strongly depend on the type and brand of ceramic, with minimum detectable dose ranging from few mGy up to several tens of mGy. A linear dose–response was observed for most of the samples. However, the luminescence signals were characterised by a significant fading, which has to be taken into account for a reliable accidental dose assessment after a radiation exposure event.     

Investigations of touchscreen glasses from mobile phones for retrospective and accident dosimetry

Touchscreen glasses of mobile phones are sensitive to ionizing radiation and have the potential of usage as an emergency dosimeter for retrospective dosimetry for the purpose of triage after a radiological accident or attack. In this study the TL glow curves and dosimetric properties of touchscreen glasses were studied in detail, such as intrinsic background dose, dose response, reproducibility, optical stability and long-term stability of the TL signal.Preliminary results are additionally presented to minimize the intrinsic background dose by mechanically removing the surface layer of the glass samples. Additionally chemical element analyses of the touchscreen glass samples were carried out to investigate the difference between glass samples which show a TL signal and samples which show neither an intrinsic zero dose signal nor a radiation induced TL signal.An irradiation trial using glass samples stored in the dark demonstrated a successful dose recovery. However, when applying a realistic, external light exposure scenario, dose underestimation was observed, even though samples were pre-bleached prior to measurement. More investigations have to be carried out in the future to solve the challenge of the low optical stability of the TL signal, if touchscreen glasses are to be used as a reliable emergency dosimeter.     

Review of optically stimulated luminescence (OSL) instrumental developments for retrospective dosimetry

This review describes 40 years of experience gained at Risø National Laboratory in the development of facilities for irradiation, thermal/optical stimulation and luminescence signal detection. These facilities have mainly been used in luminescence dating and nuclear accident dosimetry. We focus especially on methods for light stimulation and irradiation, and developments of new portable TL/OSL readers for determining doses directly in the field on both Earth and the planet Mars.     

EPR spectroscopy of radiation-induced centers in tooth enamel and its application for retrospective dosimetry in chernobyl case

A specific EPR tooth enamel dosimetry is discussed which appears to have genuine utility in retrospective dosimetry. The sample preparation technology, digital form of the native background and radiation-induced signals, and their separation from the experimentally observed spectrum are discussed. The possibility of dose estimation from the single initial EPR spectrum of randomly irradiated teeth and the uncertainty of such evaluation are discussed. The method has been used for dose reconstruction of a group of people irradiated due to the Chernobyl accident, and some results are presented.     

An international perspective on radiological threats and the need for retrospective biological dosimetry of acute radiation overexposures

The widespread use of ionizing radiation sources (machine-generated or from the decay of radioactive materials) across many disciplines including medicine, industry, and academia, has led to hundreds of instances in which one or more persons received an acute radiation overexposure. Successful medical diagnosis and management of these victims rested in part on a rapid, accurate determination of absorbed dose, which in many cases must be retrospective, due to the paucity of useful dosimetry data. This has led to the development of a number of biological dosimetry techniques to determine absorb dose retrospectively. The frequency of these accidental overexposures, however, has failed to serve as the impetus for the development of a cadre of experts in this field and an expansion in the number and availability of centers to perform the more sophisticated analysis necessary to accurately determine absorbed dose. Meanwhile, the world has seen an increase in the number of lethal terrorist events with time and there is realistic concern that the perpetrators of these events strongly desire to employ the specter of acute radiation overexposure in the future to induce mass panic in their target population. To that end, if any of these organizations achieves success, the existing capacity for rapid, accurate retrospective determination of absorbed dose may be overwhelmed, resulting in sub-optimal outcomes for the victims of such an event and potential mismanagement of medical resources designated for their care. This paper reviews existing techniques for retrospective biological dosimetry and diagnosis in relation to past experiences with overexposures, explores potential malevolent overexposure scenarios, and examines the need for public authorities to enhance national capabilities in light of the growing risk of an incident that will result in multiple acute radiation overexposures.     

Limits of retrospective accident dosimetry by EPR and TL with natural materials

The radiation response of natural materials and domestic articles was investigated by EPR and TL to select suitable materials for retrospective dose assessment in accident dosimetry. The thermal stability and the influence of UV-exposure to the radiation-induced EPR centres were investigated. Based on a required precision of ±20% for dosimetry the lower limits of applicability of the materials were determined. The lowest dosimetry limits of 0.5 Gy were found using sugar, boiler scale and egg shells by EPR and 0.3 Gy by using TL with boiler scale. A list of materials found not to be applicable for retrospective radiation accident EPR dosimetry is also given.     

The role of chemical reactions in the Chernobyl accident

It is shown that chemical reactions played an essential role in the Chernobyl accident at all of its stages. It is important that the reactor before the explosion was at maximal xenon poisoning, and its reactivity, apparently, was not destroyed by the explosion. The reactivity release due to decay of Xe-235 on the second day after the explosion led to a reactor power of 80–110 MW. Owing to this power, the chemical reactions of reduction of uranium, plutonium, and other metals at a temperature of about 2000°C occurred in the core. The yield of fission products thus sharply increased. Uranium and other metals flew down in the bottom water communications and rooms. After reduction of the uranium and its separation from the graphite, the chain reaction stopped, the temperature of the core decreased, and the activity yield stopped.     

On the use of Pd filters on proton conducting SOFC ceramics

Ceramic proton conductors are materials which conduct protons under an applied electric field and permit the construction of a SOFC in analogy to the oxygen ion conductor 8YSZ. Such protonic ceramic fuel cells have been labelled PCFCs to distinguish them from the standard SOFCs. PCFCs have several advantages when compared with standard SOFCs. First, there is no water contamination of the fuel gas. Second, the protonic conductivity may be higher in the intermediate temperature range (550 to 700 °C). Also, the activation energy for proton migration is much lower than that of oxygen ion conduction. In addition, internal reforming is also possible permitting the use of natural gas. An intriguing possibility is the use of palladium filters on the fuel side which only permit the diffusion of protons to the filter-electrolyte interface. This may reduce undesirable mixing of the fuel and the oxygen on either side of the electrolyte. In this work, it is shown that the entry of protons from the Pd into the ceramic conductor is straightforward. Prototype test PCFCs are shown to operate as required. To test the Pd - ceramic proton conductor system a study was undertaken using Pd tubes which were coated with thin layers of the proton conducting ceramics. When flushing the tube insides with hydrogen and exposing the outsides to air, Nernst voltages of such electrochemical cells could be recorded as a function of temperature. The present rather preliminary work, however, was hampered by leakage of the thin film HTPC's. Thus, the theoretical Nernst voltages were not attained. Paper presented at the 9th EuroConference on Ionics, Ixia, Rhodes, Greece, Sept. 15 – 21, 2002.     

Iron-containing atmospheric aerosols in the Chernobyl fallout

Mössbauer spectroscopy was applied to determine the composition and the iron concentration in the atmospheric aerosols contaminated in Sofia, Bulgaria after the Chernobyl accident. The results confirm the major conclusion of the Kopcewiczs for Poland, i.e. that in the initial filters, collected during the contaminating fallout (30.04–05.05.1986), the iron concentration was highest, 3.69 μg/m³ and that magnetite Fe₃O₄ was present. For the following days a change in the chemical composition including the presence of α-Fe₂O₃, α-FeOOH and γ-FeOOH as well as the absence of magnetite, was detected. Input of industrial iron contamination was negligible since the nearby steel plant had worked at minimum power due to official holidays. Unfortunately, Mössbauer spectroscopy studies only, do not allow a definite conclusion about an increase of the isotope abundance of ⁵⁷Fe in the Chernobyl fallout.     

Protocol for emergency EPR dosimetry in fingernails

There is an increased need for after-the-fact dosimetry because of the high risk of radiation exposures due to terrorism or accidents. In case of such an event, a method is needed to make measurements of dose in a large number of individuals rapidly and with sufficient accuracy to facilitate effective medical triage. Dosimetry based on EPR measurements of fingernails potentially could be an effective tool for this purpose. This paper presents the first operational protocols for EPR fingernail dosimetry, including guidelines for collection and storage of samples, parameters for EPR measurements, and the method of dose assessment. In a blinded test of this protocol application was carried out on nails freshly sampled and irradiated to 4 and 20 Gy; this protocol gave dose estimates with an error of less than 30%.     

The role of TL dosimetry in estimating patient doses

A system of determining entrance surface doses (ESDs) from diagnostic X-ray examination is described. It is shown that the radiation yield calibrations of X-ray units (μGym²mAs⁻¹) can be based on very simple measurements with TL dosimeters. Comparisons of determined ESDs with the guidelines of international organizations are carried out with the aim of demonstrating the idea of how these values can be utilized in limiting patient doses.