Analysis of EPR tooth enamel spectra exposed to combined radiation and mechanical effects

In the EPR spectra of tooth enamel samples exposed to sequential radiation and mechanical effect, the intensity of the signal in the spectra of tooth enamel samples exposed to sequential mechanical and radiation effects exceeded the amplitude of a signal in enamel samples that were only exposed to radiation. The increased dosimetric signal can be explained by superposition of mechanically and radiation-induced signals. The contribution of the mechanically induced component to the individual dose load reconstructed by EPR-spectra of tooth enamel has been evaluated.     

Spectral analysis of paramagnetic centers induced in human tooth enamel by x-rays and gamma radiation

Based on study of spectral and relaxation characteristics, we have established that paramagnetic centers induced in tooth enamel by x-rays and gamma radiation are identical in nature. We show that for the same exposure dose, the intensity of the electron paramagnetic resonance (EPR) signal induced by x-radiation with effective energy 34 keV is about an order of magnitude higher than the amplitude of the signal induced by gamma radiation. We have identified a three-fold attenuation of the EPR signal along the path of the x-radiation from the buccal to the lingual side of a tooth, which is evidence that the individual had undergone diagnostic x-ray examination of the dentition or skull. We have shown that the x-ray exposure doses reconstructed from the EPR spectra are an order of magnitude higher than the applied doses, while the dose loads due to gamma radiation are equal to the applied doses. The data obtained indicate that for adequate reconstruction of individual absorbed doses from EPR spectra of tooth enamel in the population subjected to the combined effect of x-radiation and accidental external gamma radiation as a result of the disaster at the Chernobyl nuclear power plant, we need to take into account the contribution to the dose load from diagnostic x-rays in examination of the teeth, jaw, or skull.     

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.     

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.     

Thermal induced EPR signals in tooth enamel

Electron paramagnetic resonance (EPR) spectroscopy was used to detect the effects of temperature on powdered human tooth enamel, not irradiated in the laboratory. Samples were heated at temperature between 350 and 450, at 600 and at 1000°C, for different heating times, between 6 min and 39 h. Changes in the EPR spectra were detected, with the formation of new signals. Possible correlation between the changes in EPR spectra and modifications in the enamel and in the mineral phase of bone detected with other techniques is discussed. The implications for dosimetric applications of signals induced by overheating due to mechanical friction during sample preparation are underlined.     

Multi-frequency EPR study of radiation-induced radicals in tooth enamel

Human tooth enamel powders, unheated as well as heated prior to X -irradiation at room temperature, have been investigated by means of Q - and W -band Electron Paramagnetic Resonance (EPR). Upon irradiation of enamel, carbonate-derived radicals are generated. The simplest acquired EPR spectra in this study consist mainly of a group of three different \hbox{CO}_3^{3-} signals, with a very weak \hbox{CO}_2^{-} contribution. The characterisation of the paramagnetic species in enamel is quite important for the reliability of EPR applications ( e.g. , EPR retrospective dosimetry). The spectra from the heated samples reveal a striking resemblance with spectra from certain irradiated synthetic apatite powders. The spin Hamiltonian parameters obtained from the computer simulations of the Q - and W -band spectra are compared with those reported in the literature.     

The Individual Form of the Background Signal in EPR Dosimetry of Tooth Enamel

The dependence of the calculated individual absorbed dose on the form factor, degree of anisotropy, and the model line width of the background component of the EPR spectrum of tooth enamel established. It is shown that an incorrect choice of the model line form for the background component can lead to inadequate evaluation of reconstructed load dose.     

Interlaboratory comparison of tooth enamel dosimetry on Semipalatinsk region: Part 1, general view

For intercomparison of methods of dose determination using electron paramagnetic resonance (EPR) spectroscopy of tooth enamel, the same sets of enamel samples were analyzed in different laboratories using similar recording parameters. The sets of samples included calibration samples irradiated in known doses, test samples irradiated to doses unknown to the participants and accidental dose samples prepared from teeth of humans affected by radioactive fallout from nuclear tests in the Semipalatinsk Nuclear Test Site in Kazakhstan. The test samples were analyzed to determine the differences in the resulting doses using different spectrometers and different spectra processing methods. The accidental dose samples were analyzed in order to test the precision of doses determined by EPR spectroscopy and to obtain more accurate values by averaging the results from different laboratories.     

Comparative EPR study CO2− radicals in modern and fossil tooth enamel

Comparative EPR investigation of CO₂⁻ radicals in modern (γ-irradiated) and fossil samples of tooth enamel was performed. The samples studied were the enamel powders and plates, the latter demonstrating an orientation dependence of EPR spectra in an external magnetic field. It was found that the ratio between the axial and orthorhombic CO₂⁻ centers amounts appears to be different for modern and fossil enamels. This ratio can be estimated by modeling of EPR spectra lineshape of powders or, in the case of plates, from the orientation dependence of EPR spectra in an external magnetic field. It was assumed that the difference between modern and fossil enamels is caused by the transformation, in the course of time, of orthorhombic CO₂⁻ centers into axial ones. The equations that describe this process were deduced. Their solutions show that the ratio between the amounts of the axial and orthorhombic centers does not depend on the dose rate. This finding can be used for the development of the method to determine the fossil enamel age avoiding the determination of the annual dose.     

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.     

A method for identification of interfering signals in EPR dating of tooth enamel

In this paper, a method for identifying interfering EPR signals in fossil tooth enamel is presented. This method consists of optimizing EPR parameters to enhance spectral resolution of the fossil signals followed by a g-factor and intensity normalized subtraction of a high-dosed, modern tooth enamel sample spectrum. By scanning the modern tooth enamel sample with the same parameters as the fossil sample, the difference spectrum of the fossil and modern irradiated tooth enamel samples can resolve numerous hyperfine and other interfering signals. This method was successfully applied to a fossil sample studied elsewhere (Grün, R., 1998a. Ancient TL 16, 51–55; Grün, R., Clapp, R., 1996. Ancient TL 14, 1–5; Martin Jonas, 1997. Ph.D. Thesis, Cambridge University; Jonas, M., Grün, R., 1997. Radiat. Meas. 27, 49–58; Vanhaelewyn et al., 2000. Appl. Radiat. Isot. 52, 1317–1326). This sample has shown discrepancies in dose estimations obtained from the power absorption curve versus those obtained from the first derivative spectra (Grün, R., 1998b. Radiat. Meas. 29, 177–193). The reason for this, and other discrepancies, are accounted for by the signals resolved using the method presented here.     

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.     

Interlaboratory comparison of tooth enamel dosimetry on Semipalatinsk region: Part 2, Effects of spectrum processing

In order to investigate the effects of spectrum processing procedures on the results of dose determination using EPR spectroscopy of human tooth enamel, spectra of the same samples measured in different laboratories in the course of the intercomparison were processed by some of the participants using their own unique procedures. Spectra of samples irradiated to known doses (calibration samples) and of samples irradiated to doses unknown to the participants (test samples) were analyzed. By comparison of the results obtained using different spectrum processing methods, it is shown that the precision of calibration and the accuracy of dose determination may be improved by appropriate choice of spectrum processing procedure.     

Retrospective dosimetry assessment using the 380 °C thermoluminescence peak of tooth enamel

The thermoluminescence (TL) response to gamma-ray irradiation of tooth enamel is reported. The tooth enamel was separated from dentine by using mechanical and physico-chemical procedures followed by grinding (grain size ∼100 μm) and etching. The TL was attributed to the recombination of radicals incorporated into or attached to the surface of hydroxyapatite crystals. The growth of the ∼380 °C TL peak with absorbed dose was examined with irradiated tooth enamel samples and reconstructed doses evaluated for tooth enamel samples from four human subjects.     

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.     

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.     

EPR and UV spectrometry investigation of sucrose irradiated with carbon particles

Solid state/EPR (SS/EPR) dosimeters of carbon ions irradiated sucrose are studied with EPR, and their water solutions – with UV spectroscopy. Doses between 20 and 200 Gy are used with linear energy transfer (LET) values for carbon ions of 63, 77, 96 and 230 keV μm^?1. After irradiation all samples show typical for irradiated sucrose EPR and UV spectra. The obtained data are compared with those previously reported for nitrogen particles and gamma rays irradiated sucrose. The identical shape of both the EPR and UV spectra of irradiated with various type radiation samples suggests that generated free radicals are not influenced by the nature of radiation. The lack of difference in the line width of the separate lines or the whole EPR spectrum, obtained for gamma and heavy particles irradiation, suggests negligible spin–spin interaction among the radiation-generated free radicals in the samples. The linear dependence of the EPR response on the absorbed dose radiation is found to be higher when generated by gamma rays, than by the same absorbed dose of heavy particles. In addition, the EPR response for carbon ions is higher than that for nitrogen ions. Water solutions of irradiated sucrose exhibit UV spectrum with absorption maximum at 267 nm, attributed to the recombination products of free radicals. The UV band intensity depends on the absorbed dose radiation. The UV spectra obtained for carbon, nitrogen and gamma rays irradiated sucrose are also compared.     

FT‐Raman investigation of human dental enamel surfaces

FT‐Raman spectra of human enamel surfaces from sound, affected (with 1 cavity) and highly affected (with at least 3 cavities) tooth samples were analyzed by principal component analysis (PCA). Major differences between the unaffected and affected tooth samples seem to arise from the structural changes along the c‐axis of hydroxyapatite, the chief crystalline component of human dental enamel. Based on Fisher index calculations, the most discriminative value was obtained for the intensity of the only Raman active ν₂PO₄³⁻ (E₁) symmetric deformation mode at 428 cm⁻¹. Moreover, these changes can be observed through the whole tooth enamel surface, establishing a predisposition to caries correlated to chemical and structural composition of tooth enamel. No spectral changes regarding the CO₃²⁻ substitution were detected by both nondestructive FT‐Raman and FTIR (Fourier transform infrared) spectroscopy of the powdered teeth samples. Copyright © 2009 John Wiley & Sons, Ltd.     

EPR-dosimetry with carious teeth

The effect of caries in EPR dosimetry of tooth enamel (in the dose range of 0–1 Gy) was investigated. The enamel of each tooth was divided into carious, non-carious and intermediate portions. The EPR signals of enamel at g = 2.0018 (dosimetric) and g = 2.0045 (native) were examined. The intensity of the dosimetric signal was the same for all three portions, while that of the native signal was higher for carious portions than for non-carious and intermediate portions. Reconstruction of the laboratory applied doses was done using all portions. Reasonable correlation between nominal and reconstructed doses was found in most cases. The effect of alkali treatment on the native and dosimetric signals of enamel was also tested. Reduction of the native signal intensity, particularly in the carious portions, was found to be the only significant effect. This resulted in a slight improvement in the accuracy of the reconstructed doses.     

Spatial distribution of radiation defects in tooth enamel

The spatial distribution of radiation defects in tooth enamel has been investigated using EPR imaging. Plates of enamel irradiated with γ rays and electrons with energy 1.2 and 3.8 MeV have been studied. A falloff of the radiation-defect concentration in the direction in which the radiation acts is detected in the electron-irradiated plates, with the slope of the falloff decreasing with increasing electron energy. The defect distribution was uniform in the γ-irradiated plates. It is shown that the study of tooth enamel by means of EPR imaging can be used to determine the type and energy characteristics of the ionizing radiation that acts on a living organism. Fiz. Tverd. Tela (St. Petersburg) 41, 1207–1209 (July 1999)