EPR dosimetry in chemically treated fingernails

By using EPR measurements of radiation-induced radicals it is possible to utilize human fingernails to estimate radiation dose after-the-fact. One of the potentially limiting factors in this approach is the presence of artifacts due to mechanically induced EPR signals (MIS) caused by mechanical stress during the collection and preparation of the samples and the so-called background (non-radiation) signal (BKS). The MIS and BKS have spectral parameters (shape, g-factor and linewidth) that overlap with the radiation-induced signal (RIS) and therefore, if not taken into account properly, could result in a considerable overestimation of the dose. We have investigated the use of different treatments of fingernails with chemical reagents to reduce the MIS and BKS. The most promising chemical treatment (20 min with 0.1 M dithiothreitol aqueous solution) reduced the contribution of MIS and BKS to the total intensity of EPR signal of irradiated fingernails by a factor of 10. This makes it potentially feasible to measure doses as low as 1 Gy almost immediately after irradiation. However, the chemical treatment reduces the intensity of the RIS and modifies dose dependence. This can be compensated by use of an appropriate calibration curve for assessment of dose. On the basis of obtained results it appears feasible to develop a field-deployable protocol that could use EPR measurements of samples of fingernails to assist in the triage of individuals with potential exposure to clinically significant doses of radiation.     

Electron paramagnetic resonance radiation dosimetry in fingernails

There is now an increased need for accident dosimetry due to the increased risk of significant exposure to ionizing radiation from terrorism or accidents. In such scenarios, dose measurements should be made in individuals rapidly and with sufficient accuracy to enable effective triage. Electron paramagnetic resonance (EPR) is a physical method of high potential for meeting this need, providing direct measurements of the radiation-induced radicals, which are unambiguous signatures of exposure to ionizing radiation. For individual retrospective dosimetry, EPR in tooth enamel is a proven and effective technique when isolated teeth can be obtained. There are some promising developments that may make these measurements feasible without the need to remove the teeth, but their field applicability remains to be demonstrated. However, currently it is difficult under emergency conditions to obtain tooth enamel in sufficient amounts for accurate dose measurements. Since fingernails are much easier to sample, they can be used in potentially exposed populations to determine if they were exposed to life-threatening radiation doses. Unfortunately, only a few studies have been carried out on EPR radiation-induced signals in fingernails, and, while there are some promising aspects, the reported results were generally inconclusive. In this present paper, we report the results of a systematic investigation of the potential use of fingernails as retrospective radiation dosimeters.     

EPR tooth dosimetry of SNTS area inhabitants

The determination of external dose to teeth of inhabitants of settlements near the Semipalatinsk Nuclear Test Site (SNTS) was conducted using the EPR dosimetry technique to assess radiation doses associated with exposure to radioactive fallout from the test site. In this study, tooth doses have been reconstructed for 103 persons with all studied teeth having been formed before the first nuclear test in 1949. Doses above those received from natural background radiation, termed “accident doses”, were found to lie in the range from zero to approximately 2 Gy, with one exception, a dose for one person from Semipalatinsk city was approximately 9 Gy. The variability of reconstructed doses within each of the settlements demonstrated heterogeneity of the deposited fallout as well as variations in lifestyle. The village mean external gamma doses for residents of nine settlements were in the range from a few tens of mGy to approximately 100 mGy.     

EPR dosimetry for actual and suspected overexposures during radiotherapy treatments in Poland

EPR dosimetry on bone samples was recently used for actual and suspected overexposures during radiotherapy treatments performed in Poland. In 2001 five breast-cancer patients undergoing radiotherapy in the Bialystok Oncology Center, Poland, were overexposed. The overexposure was due to a defective safety interlock and an obsolete safety system of the linear accelerator. For the three most exposed patients, pieces of rib bones removed during surgical reconstruction of the chest wall and skin transplantation allowed an estimation of the accident doses by electron paramagnetic resonance (EPR) spectrometry. The doses delivered during the accident were as high as 60–80 Gy. In 2005, a patient treated in Kielce Holy Cross Cancer Center exhibited similar deep necroses of the chest wall but 6 years following a “standard upper mantel fields” radiotherapy for Hodgkin's disease. In order to investigate the possible late effect of an overexposure as necrosis origin, the delivered dose was afterward estimated by EPR dosimetry performed on a rib sample.     

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.     

Quantum Encryption Protocol Based on Continuous Variable EPR Correlations

A quantum encryption protocol based on Gaussian-modulated continuous variable EPR correlations is proposed. The security is guaranteed by continuous variable EPR entanglement correlations produced by nondegenerate optical parametric amplifier (NOPA). For general beam splitter eavesdropping strategy, the mutual information Ⅰ(α, ε)between Alice and Eve is calculated by employing Shannon information theory. Finally the security analysis is presented.     

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.     

Quantum Encryption Protocol Based on Continuous Variable EPR Correlations

A quantum encryption protocol based on Gaussian-modulated continuous variable EPR correlations is proposed. The security is guaranteed by continuous variable EPR entanglement correlations produced by nondegenerate optical parametric amplifier （NOPA）. For general beam splitter eavesdropping strategy, the mutual information I（α, ε） between Alice and Eve is caJculated by employing Shannon information theory. Finally the security analysis is presented.     

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.     

EPR of gamma irradiated solid sucrose and UV spectra of its solution. An attempt for calibration of solid state/EPR dosimetry

A simple new approach for independent calibration of solid state/EPR (SS/EPR) dosimetry system is reported. It is based on the fact that: (i) gamma-irradiation of solid sucrose (sugar) induces stable EPR detectable free radicals accompanied by UV detectable brown colour stable in the solid state and in solution; (ii) both the EPR intensity of gamma-irradiated solid sucrose and its solution UV absorbance linearly depend on the absorbed dose high energy radiation and may be independently used for dosimetric purpose; (iii) UV spectrometers are calibrated. The correlation between EPR response and absorbed dose radiation of solid sucrose and UV absorption of its solutions is used in the present communication for calibration purpose. The procedure of sucrose extraction from sucrose-paraffin dosimeters is described. The calibration procedure may be applied to any other (alanine, self-calibrated, etc.) SS/EPR dosimeters, simultaneously irradiated with sucrose.     

EPR of carbonate derived radicals: Applications in dosimetry, dating and detection of irradiated food

After exposure of biological (tooth enamel, bone, …) and synthetic apatites to ionizing radiation, the so-called “asymmetric EPR signal nearg = 2” is formed. Although this signal is being used in EPR dosimetry, dating and detection of irradiated food for many years already, its composite character and the precise nature of the radicals contributing to the spectrum are still insufficiently known and/or recognized. For some fifteen years already, the EPR group in Ghent is gaining extensive experience on the radicals present in calcified tissues and model systems like synthetic apatites, calcites and single crystals doped with carbonate. It will be shown that the majority of radicals in calcified tissues are carbonate derived, e.g., CO ₂ ^? , CO ₃ ^? , CO ₃ ^3? while also phosphate derived radicals like PO ₄ ^2? and oxygen species (O^?, O ₃ ^? ) have been identified with EPR and/or ENDOR. For the EPR applications mentioned above, the most important type of radicals is CO ₂ ^t- (g values ranging from 2.0035 to 1.9970). A second type of radicals which is very intriguing but still badly known, exhibits a spectrum atg values around 2.0045. It is very apparent in tooth enamel below doses of 1 Gy, it has been observed in certain fossil teeth in a very prominent way and also in irradiated food containing bone (e.g., frog legs). It will be shown that the organic origin of this signal can be questioned. The importance of other radicals like CO ₃ ^3t- and CO ₃ ^t- for EPR applications will also be discussed.     

EPR dosimetry sensitivity enhancement by detection of rapid passage signal of the tooth enamel at low temperature

The four-fold improvement of EPR signal-to-noise ratio for radiation-induced paramagnetic centres in comparison with a conventional way is achieved by detection of the tooth enamel EPR signal at 77 K and rapid passage conditions.     

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.     

Radical formation in lithium trifluoromethane-sulfonate for ESR dosimetry

Lithium trifluoromethane-sulfonate (Li-TFMS:CF₃SO₃Li) irradiated by γ-rays showed an electron spin resonance (ESR) powder spectrum having the rhombicg-factor ofg _xx = 2.0259 ± 0.0005,g _yy = 2.0112 ± 0.0005 andg _zz = 2.0025 ± 0.0005 and a triplet hyperfine coupling constant ofA _xx/gβ= 0.8 ± 0.15 mT.A _yy andA _zz are not obtained because of the broadened spectrum. The energy levels,g-factor,A _xx/gβ and optical absorption spectrum of several conceivable radicals such as C^⋅F₂SO₃Li, CF₃-S-O^⋅ and CF₃-S-O-O^⋅ have been calculated by softwares MOPAC-V2 and Gaussian-98 based on ROHF (Restricted Hatree-Fock for open shell molecule). The most probable radical was ascribed to CF₃-SO^⋅ from both calculated and experimental results. The response to γ-ray dose and the thermal stability have been studied in addition to the effect of UV illumination for possible use of the signal intensity in ESR dosimetry. The obtained number of free radicals per 100 eV (G-value) was 1.23 ± 0.40.     

Electrochemical etching technique for neutron dosimetry

In the present work we have employed allyl diglycol carbonate (CR-39) and cellulose triacetate (CTA) plastic for detection of neutron recoil tracks without radiator. For CR-39, the results reveal that registration efficiency is a function of duration of chemical pre-etching and the best results are obtained with chemical pre-etching of 3 hours. It was also investigated that the ac field strength of 28 kV/cm having 2.5 kHz frequency was optimum for revelation of tracks. Interestingly the sensitivity is fluence dependent and it was constant up to a fluence of about 10⁸ n/cm². The sensitivity abruptly decreased with increased fluence. At optimum experimental conditions the minimum detection limit for CR-39 was found to be 0.47 mSv. For CTA, the tracks have been revealed by electrochemical etching (ECE) only and the minimum detection limit was found to be 0.85 mSv at optimum experimental parameters.      

Planar microresonators for EPR experiments

EPR resonators on the basis of standing-wave cavities are optimised for large samples. For small samples it is possible to design different resonators that have much better power handling properties and higher sensitivity. Other parameters being equal, the sensitivity of the resonator can be increased by minimising its size and thus increasing the filling factor. Like in NMR, it is possible to use lumped elements; coils can confine the microwave field to volumes that are much smaller than the wavelength. We discuss the design and evaluation of EPR resonators on the basis of planar microcoils. Our test resonators, which operate at a frequency of 14 GHz, have excellent microwave efficiency factors, achieving 24 ns pi/2 EPR pulses with an input power of 17 mW. The sensitivity tests with DPPH samples resulted in the sensitivity value 2.3 x 10(9) spins.G(-1) Hz(-1/2) at 300 K.