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.     

ISS protocol for EPR tooth dosimetry

The accuracy in Electron Paramagneetic Resonance (EPR) dose reconstruction with tooth enamel is affected by sample preparation, dosimetric signal amplitude evaluation and unknown dose estimate. Worldwide efforts in the field of EPR dose reconstruction with tooth enamel are focused on the optimization of the three mentioned steps in dose assessment. In the present work, the protocol implemented at ISS in the framework of the European Community Nuclear Fission Safety project “Dose Reconstruction” is presented. A combined mechanical–chemical procedure for ground enamel sample preparation is used. The signal intensity evaluation is carried out with powder spectra simulation program. Finally, the unknown dose is evaluated individually for each sample with the additive dose method. The unknown dose is obtained by subtracting a mean native dose from the back-extrapolated dose. As an example of the capability of the ISS protocol in unknown dose evaluation, the results obtained in the framework of the 2nd International Intercomparison on EPR tooth enamel dosimetry are reported.     

Advances towards using finger/toenail dosimetry to triage a large population after potential exposure to ionizing radiation

Rapid and accurate retrospective dosimetry is of critical importance and strategic value for the emergency medical response to a large-scale radiological/nuclear event. One technique that has the potential for rapid and accurate dosimetry measurements is electron paramagnetic resonance (EPR) spectroscopy of relatively stable radiation-induced signals (RIS) in fingernails and toenails. Two approaches are being developed for EPR nail dosimetry. In the approach using ex vivo measurements on nail clippings, accurate estimation of the dose-dependent amplitude of the RIS is complicated by the presence of mechanically-induced signals (MIS) that are generated during the nail clipping. Recent developments in ex vivo nail dosimetry, including a thorough characterization of the MIS and an appreciation of the role of hydration and the development of effective analytic techniques, have led to improvements in the accuracy and precision of this approach. An in vivo nail dosimetry approach is also very promising, as it eliminates the problems of MIS from the clipping and it has the potential to be an effective and efficient approach for field deployment. Two types of EPR resonators are being developed for in vivo measurements of fingernails and toenails.     

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.     

Optimisation of an EPR dosimetry system for robust and high precision dosimetry

Clinical applications of electron paramagnetic resonance (EPR) dosimetry systems demand high accuracy causing time consuming analysis. The need for high spatial resolution dose measurements in regions with steep dose gradients demands small sized dosimeters. An optimization of the analysis was therefore needed to limit the time consumption. The aim of this work was to introduce a new smaller lithium formate dosimeter model (diameter reduced from standard diameter 4.5 mm to 3 mm and height from 4.8 mm to 3 mm). To compensate for reduced homogeneity in a batch of the smaller dosimeters, a method for individual sensitivity correction suitable for EPR dosimetry was tested. Sensitivity and repeatability was also tested for a standard EPR resonator and a super high Q (SHQE) one. The aim was also to optimize the performance of the dosimetry system for better efficiency regarding measurement time and precision. A systematic investigation of the relationship between measurement uncertainty and number of readouts per dosimeter was performed. The conclusions drawn from this work were that it is possible to decrease the dosimeter size with maintained measurement precision by using the SHQE resonator and introducing individual calibration factors for dosimeter batches. It was also shown that it is possible reduce the number of readouts per dosimeter without significantly decreasing the accuracy in measurements.     

Radiation Dosimetry Using Alanine and Electron Paramagnetic Resonance (EPR) Spectroscopy: A New Look at an Old Topic

The detection and quantification by electron paramagnetic resonance (EPR) spectroscopy of stable radicals formed in alanine by exposure to γ-radiation is used as a secondary standard for radiation dosimetry measurements, even though the EPR signal is actually derived from >1 radical with different spectral properties. For high radiation doses, microwave power saturation and spectral linewidths are both dependent on the received dose, and result in non-linear calibration curves. Furthermore, using a high-sensitivity microwave cavity, the power at which EPR signal saturation commences is ~0.3–0.4 mW for samples with irradiation doses ≤10 kGy; these values are an order of magnitude lower than those normally used in alanine dosimetry. In addition, the central peak of the first derivative spectrum, the height of which is commonly used in dosimetry measurements, is the most susceptible to microwave power saturation. Therefore, for high-level dosimetry we now recommend that analyses be performed under non-saturating conditions, and that the spectral acquisition parameters should be determined with a standard irradiated to ≤10 kGy to eliminate any intensity problems associated with variable saturation characteristics. At low radiation doses, variations in spectral saturation characteristics are negligible, and partially saturating conditions along with modulation amplitudes much higher than those normally used can reliably produce improved signal-to-noise ratios and allow extension of the methodology to practical working limits of ~0.1–0.2 Gy.     

Radiation dose reconstruction from L-band in vivo EPR spectroscopy of intact teeth: Comparison of methods

In vivo EPR tooth dosimetry is a more challenging problem than in vitro EPR dosimetry because of several potential additional sources of variation associated with measurements that are made in the mouth of a living subject. For in vivo measurement a lower RF frequency is used and, unlike in the in vitro studies, the tooth cannot be processed to optimize the amount and configuration of the enamel that is measured. Additional factors involved with in vivo measurements include the reproducibility of positioning the resonator on the surface of the tooth in the mouth, irregular tooth geometry, and the possible influence of environmental noise. Consequently, in addition to using the theoretical and empirical models developed for analyzing data from measurements of teeth in vitro, other unconventional and more robust methods of dose reconstruction may be needed. The experimental parameter of interest is the peak-to-peak amplitude of the spectrum, which is correlated to the radiation dose through a calibration curve to derive the reconstructed dose. In this study we describe and compare the results from seven types of computations to measure the peak-to-peak amplitude for estimation of the radiation induced signal. The data utilized were from three sets of in vivo measurements of irradiated teeth. Six different teeth with different doses were placed in the mouth of a volunteer in situ and measurements of each tooth were carried out on three different days. The standard error of dose prediction (SEP) is used as a figure of merit for quantifying precision of the reconstruction. We found that many of the methods gave fairly similar results, with the best error of prediction resulting from a computation based on a Lorentzian line model whose center field corresponds to the known parameter of the radiation-induced EPR spectra of teeth, with corrections from a standard sample that was measured as part of the data acquisition scheme. When the results from the three days of measurement were pooled, the SEP decreased dramatically, which suggests that one of the principal sources of variation in the data is the ability to precisely standardize the measurements conditions within the mouth. There are very plausible ways to accomplish improvements in the existing procedures.     

Feasibility of Q-Band EPR Dosimetry in Biopsy Samples of Dental Enamel, Dentine and Bone

Electron paramagnetic resonance (EPR) dosimetry of tooth enamel in X-band has been established as a suitable method for individual reconstruction of doses 0.1 Gy and higher. The objective was to demonstrate the feasibility of using Q-band EPR in small biopsy tooth enamel samples to provide accurate measurements of radiation doses. Q-band spectra of small (<10 mg) irradiated samples of dentine and bone were studied to investigate the possibility of using Q-band EPR for dose measurements in those materials if there are limited amounts of enamel available, and there is no time for the chemical sample preparation required for accurate X-band measurements in dental enamel. Our results have shown that Q-band provides accurate measurements of radiation doses higher than 0.5 Gy in tooth enamel biopsy samples as small as 2 mg. Q-band EPR spectra in powdered dentine and bone demonstrated significantly higher resolution and sensitivity than in conventional X-band measurements.     

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 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.     

EPR在体测量专用调制磁场驱动装置

利用电子顺磁共振（electron paramagnetic resonance,EPR）在体测量人牙齿可以实现无损伤地快速评估人体辐射剂量,具有实际应用价值.本文针对EPR在体测量牙齿剂量的应用特点,研制了专用调制磁场驱动装置,包括功率放大器、调制磁场激励线圈、调制频率设定模块、感应型调制幅度显示模块等.功率放大器采用脉冲功率放大方式取代传统的线性放大方式,用多N-MOSFET管H桥电路,功率容量大、效率高、结构简单,且调制频率设定自如.实验结果表明：（1）此装置可在大于9 cm磁极间距的中心样品位置产生调制幅度为0~0.9 mT的调制磁场,调制频率为10~100 kHz;（2）用该装置与EPR在体测量谱仪配合使用,可以明显观测到1,1-二苯基-2-三硝基苯肼（1,1-diphenyl-2-picrylhydrazyl,DPPH）样品谱线调制增宽过程以及辐射诱发的整体牙齿中的自由基信号,验证了该装置的高调制效率和实用性.     

Experimental Procedures for Sensitive and Reproducible In Situ EPR Tooth Dosimetry

In vivo electron paramagnetic resonance (EPR) tooth dosimetry provides a means for non-invasive retrospective assessment of personal radiation exposure. While there is a clear need for such capabilities following radiation accidents, the most pressing need for the development of this technology is the heightened likelihood of terrorist events or nuclear conflicts. This technique will enable such measurements to be made at the site of an incident, while the subject is present, to assist emergency personnel as they perform triage for the affected population. At Dartmouth Medical School this development is currently being tested with normal volunteers with irradiated teeth placed in their mouths and with patients who have undergone radiation therapy. Here we describe progress in practical procedures to provide accurate and reproducible in vivo dose estimates.     

Effect of spectrum processing procedure on the linearity of EPR dose reconstruction in tooth enamel

Electron Paramagnetic Resonance (EPR) spectroscopy with tooth enamel is a widely used method of dosimetry. The accuracy of EPR tooth dosimetry depends on the spectrum processing procedure, the quality of which, in its turn, relies on instrumental noise and the signals from impurities. This is especially important in low-dose evaluation. The current paper suggests a method to estimate the accuracy of a specific spectrum processing procedure. The method is based on reconstruction of the radiation-induced signal (RIS) from a simulated spectrum with known RIS intensity. The Monte Carlo method was used for the simulations. The model of impurity and noise signals represents a composite residual spectrum (CRS) obtained by subtraction of the reconstructed RIS and the native background signal (BGS) from enamel spectra measured in HMGU (Neuherberg, Germany) and IMP (Yekaterinburg, Russia). The simulated spectra were deconvoluted using a standard procedure. The method provides an opportunity to compare the simulated “true” RIS with reconstructed values. Two modifications of the EPR method were considered: namely, with and without the use of the reference Mn²⁺ signals. It was observed that the spectrum processing procedure induces a nonlinear dose response of the reconstructed EPR amplitude when the height of the true RIS is comparable with the amplitudes of noise-like random splashes of CRS. The area of nonlinearity is below the limit of detection (DL). The use of reference Mn²⁺ signals can reduce the range of nonlinearity. However, the impact of the intensities of CRS random signals on nonlinearity is two times higher than the one observed when the reference signals were not used. The reproducibility of the software response is also dependent on both the amplitude of the CRS and the use of a reference signal, and it is also two times more sensitive to the amplitude of the CRS. In most EPR studies, all of the data are used, even those for which the dose value is lower than the DL. This study shows that low doses evaluated with the help of linear dose–response can be significantly overestimated. It is recommended that linear dose response calibration curves be constructed using only data above the DL. Data below the DL should be interpreted cautiously.     

The second international intercomparison on EPR tooth dosimetry

Eighteen international EPR laboratories participated in the second intercomparison programme. Each participant had to prepare enamel samples and evaluate the absorbed dose from molars that were irradiated in vitro in the range 0–1000 mGy. The objective of the programme was to bring together all methods which are currently applied by different laboratories for EPR dose reconstruction and to demonstrate the present state of dosimetry. An overview of the essential features of the different methods is presented. The current accuracy of EPR tooth enamel dosimetry under defined conditions of irradiation is evaluated.     

Dose reassessment by using PTTL method in MTS-N (LiF:Mg,Ti) thermoluminescent detectors

The thermoluminescent (TLD) method is one of the most commonly used in dose measurements in radiation protection dosimetry. Due to its many advantages this method is widely spread. However, TLD has especially one disadvantage which is very inconvenient: the dose information in already read detectors is erased and in routine standard way the dose can not be reassessed. The positive is that this shortcoming can be eliminated by applying UV radiation. After first readout the same detector can be subjected to UV exposure and then read once again to reassess the dose.This method for reassessment of dose is based on phototransferred thermoluminescence (PTTL). In an irradiated TL detector deep traps are not emptied during the first readout. During exposure to UV, electrons are transferred from deep traps to shallower dosimetric traps. This TL signal emerging during the second readout following UV illumination is called phototransferred thermoluminescence.A method for reassessment of dose in a previously readout TLD is presented in this work. Experiments show that the method works well within region of doses between 5 and 50 mGy, but could be applied for higher doses as well. The efficiency of dose reassessment reaches about 17 percent of the first readout.The method could be a noticeable improvement in TLD dosimetry, giving more opportunities for better control and reliability of measurements.     

Emergency EPR dosimetry technique using vacuum-stored dry nails

Human finger- and toenails have been tested with an X-band EPR technique for different conditions of nail storage. The main radiation-induced signal at g = 2.005 demonstrated good stability if the samples were stored in a vacuum at room temperature after nail harvesting and irradiation. On the basis of this phenomenon, a new protocol is proposed to use the nails as possible emergency EPR dosimeters. The dosimetry protocol was tested on laboratory-exposed samples and demonstrated the ability to recover doses in the region 0–10 Gy with an estimated uncertainty of approximately 0.3–0.4 Gy for doses in the range <2 Gy, increasing to 0.6–0.7 Gy for doses in the range 5–10 Gy.     

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.     

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.     

Signal processing for radiation dosimetry using EPR in dental enamel: comparison of three methods

We are reporting an alternative method of extracting useful dose information from complex EPR spectra of dental enamel. Digital differentiation of the initial first derivative spectrum followed by filtering is used to clearly distinguish the radiation-induced signal from the native background signal. The peak-to-peak height of the resulting second derivative of the signal is then measured as an indication of absorbed dose. This method does not require preliminary elimination of the native background signal, and is not effected by any uncertainty in the determination of the background signal or by errors resulting from the subtraction of two signals of comparable magnitude. Ten enamel samples were irradiated with known doses in the range of 250–10⁵ mGy. There was agreement for all the samples, within the typical experimental error of ±10% for EPR dosimetry in dental enamel, between the doses determined by two common techniques using native signal subtraction and the doses determined by the new second derivative method proposed here.